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                              Contents

Acknowledgments	iii
Introduction	1
Chapter 1.  Gasoline-fueled Spark-ignition Engines	5
Chapter 2.  Pollutant Formation—General Effects	11
      2.1. Fuel Complexity	ill
      2.2. Combustion Complexity	15
Chapter 3.  Pollutant Formation—Specific Effects	20
      3.1. Effect of Flame Quenching	21
      3.2. Effect of Oxygen Content on CO Formation	22
      3.3. Effect of Temperature on NO Formation	22
Chapter 4.  Pollutant Control Approaches	24
      4.1. Preventive Techniques	24
           4.1.1. Combustion Chamber Redesign for HC
                  Minimization	24
           4.1.2. Fuel Control for CO Minimization	25
           4.1.3.  Temperature Control for NO Minimization	25
      4.2. Remedial Techniques	27
           4.2.1.  Supplementary Air Oxidation	27
           4.2.2. Catalytic Conversion	30
      4.3. Interaction Complications	37
Appendixes	39
      Appendix 1.  Comparison of Four-stroke Spark-ignition and
           Compression-ignition Engines	41
           Speed and Power Output Control	41
           Fuel Properties	42
           Fuel Introduction	42
           Combustion Initiation	43
           Pollutant Formation	43
      Appendix 2.  Hydrocarbon Classes	47
           Paraffin (Alkane) Hydrocarbons	48
           Isoparaffin (Alkane) Hydrocarbons	48
           Cycloparaffin (Alkane) Hydrocarbons	49
           Olefin (Alkene) Hydrocarbons	49
           Hydrocarbons with Six Carbon Atoms	50
           Oxygenated Organic Compounds	51

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                                Figures

Figure 1.  Engine Block and Head (cross-section)	5
Figure 2.  Engine Block and Manifolds...	6
Figure 3.  Spark-ignition Phases	7
Figure 4.  Molecular Structure of Selected Hydrocarbons	11
Figure 5.  Flame Quenching	21
Figure 6.  Surf ace/Volume Ratio  Changes	25
Figure 7.  Internal Exhaust  Gas Recirculation (Valve Overlap)	27
Figure 8.  External Exhaust Gas Recirculation	'.	28
Figure 9.  Aspirated Air'Injection	29
Figure 10. Forced Air Injection	30
Figure 11. Exhaust Composition	35
Figure 12. Closed Loop Fuel Flow Control System	36
                                Tables

Table 1. Relationship of Combustion Phase and Piston Stroke	6
Table 2. Hydrocarbon Compounds and Properties	13
Table3. Exhaust Pollutants	20
Table 4. O2 & CO Concentration by Air/Fuel Ratio.	33
11

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                          Acknowledgments

      The preparation of this synopsis involved several revisions which
affected both form and content.  The changes incorporated in the successive
drafts resulted in significant improvements; such as, (a) the addition of
essential material that was initially overlooked, (b) the clarification of some of
the original technical explanations, (c) the reduction of the number of pages
in the original text by the use an appendix for discussions that were judged to
be too detailed to be of general interest, and (d) the addition of technical
drawings to clarify material.  These improvements resulted  from comments
and suggestions made by several individuals who graciously agreed to review
the early drafts.  These reviewers very generously devoted the time and
energy which the detailed reviews required with no motivation other than
their desire to be helpful. Consequently, an expression of appreciation for the
efforts of the following individuals is essential and most appropriate: R. J.
Bergin, Gay MacGregor, John L. WeRrly, and Kenneth L. Zerafa.
      In addition, thanks must be extended to the following individuals who
volunteered to review the later drafts and provided comments  which
permitted the further refinement of this synopsis: Judy F. Carmickle,
William B. Clemmens, Charles D. Cole, John M. German, Barry S. Mclntyre,
Jeff T. Prince, and Clifford D. Tyree.
      Lastly, thanks to editor Kathy E. Carter for the final refinements to the
document and to illustrator Frank Lamitola for creating the drawings which
add so much clarity to the text.
                                                         John W. Bozek
                                                       November 2, 1990

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                             Introduction

      The pollutant formation and control information provided in this
synopsis is specifically applicable to gasoline-powered, four-stroke,
reciprocating piston, spark-ignition motor vehicle engines.  This information
is presented with the hopeful intention of providing the non-technical reader
with a basis  for understanding the applicable chemical and physical
phenomena.  Consequently, the discussion of these phenomena emphasizes
cause and effect relationships which may not be obvious to a reader who does
not have an  engineering background and, hence, might be overlooked by
such a reader if such highlighting was not attempted.
      For example, the discussion of spark-ignition engine  construction and
operation in Chapter 1 calls attention to the correspondence between
      •  the four strokes of the cycle and the four phases of the associated
         combustion process  and  -
      •  the effects of the cycle and the process on the related pollutant
         formation mechanisms.
      Chapter 2 discusses pollutant formation on an overall basis by relating
two factors,  fuel complexity and combustion complexity, to  the generalized
effects on the energy generation process and on the pollution formation
mechanisms. Fuel complexity is discussed by relating the many different
kinds of hydrocarbon compounds present in gasoline to the effects of the
physical properties of the compounds on the combustion process.
Combustion complexity is discussed in Chapter 2 in terms of the variations in
the structure and operation of the engine. \These variations affect the
combustion  of the fuel by limiting the use of\ the chemical energy in the fuel
for developing mechanical energy needed for operating the vehicle.
        This chapter also provides an understanding of how one set of
complexities affects the other. The relationship between fuel complexity and
combustion  complexity is shown by pointing out that—
      •  using a complex fuel (with different types pf hydrocarbons), instead
         of  a simple fuel (with one type of hydrocarbon), complicates the
         combustion process  and
      •  using a complex combustion process  (involving the discontinuous
         burning of combustible air/fuel mixtures in an enclosed chamber),

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Formation and Control of Combustion Pollutants


         instead of a simple process (involving the continuous open-flame
         burning), complicates the effective utilization of the fuel.

      The emphasis on relationships is continued in Chapter 3 which
discusses pollutant formation in detail by highlighting the differences
between the various cause and effect events accounting for the presence of
hydrocarbons (HC), carbon monoxide (CO), and nitric  oxide (NO) in the
exhaust. This discussion stresses the following:
      •  During the combustion process, most of the  hydrogen and carbon
         atoms in the fuel hydrocarbon molecules are separated from each
         other and oxidized to water vapor (H2O) and carbon dioxide (CO2),
         respectively.
      •  A small fraction  of the fuel molecules undergo less complete
        . reactions which result in the carbon atoms being partially oxidized
         to carbon monoxide and the  hydrogen atoms associating with each
         other to form diatomic hydrogen molecules.
      •  Another small fraction of the fuel molecules are more or less
         excluded from the combustion process, primarily as a result of
         flame quenching. These molecules pass through the combustion
         chamber either completely unaltered, restructured in some way, or
         converted into various forms of oxygenated organic compounds.
      •  NO molecules in the exhaust are not directly products of the
         combustion process but, rather, are products of a high temperature
         side reaction which  involves the disassociation of some of the
         atmospheric nitrogen molecules, the oxidation of the liberated
         nitrogen atoms to NO, and the subsequent conversion of the NO to
         other nitrogen oxides, such as nitrogen dioxide (NO2), when the
         exhaust gases are released to the atmosphere.

      In a comparable way, Chapter 4  discusses pollution control by
associating several techniques presently used with the two possible control
approaches, preventive and remedial. Each technique is related to the
pollutant formation phenomena discussed in Chapter 3.

      Engine combustion chamber redesign is discussed as an HC preventive
technique which reduces flame quenching and, hence, minimizes the
number of fuel molecules that are isolated from the combustion process.
Fuel flow control is discussed as a CO preventive  technique which controls
fuel input to ensure that the oxygen available in the ingested air is adequate
to maximize the oxidation  of the fuel HC molecules. Exhaust gas
recirculation is discussed as an NO preventive technique which limits the

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                                                              Jitroduction

combustion chamber temperature to minimize the oxidation of atmospheric
nitrogen.
      Supplementary air injection is discussed as a remedial technique which
adds air to the hot exhaust gases so that the additional oxygen can react with
the HC and CO molecules that exit the combustion chamber.  Catalytic
conversion is discussed as a remedial technique which oxidizes HC and CO
molecules and reduces NO molecules.  This discussion is focused on closed
loop fuel control systems which use  three-way catalysts, lambda sensors, and
electronic control units to maintain proportions of air and fuel close to the
chemically correct, "stoichiometric," ratio.
      The final relationships highlighted in Chapter 4 are the possible
interactions between the  various control techniques.  This discussion
illustrates the fact that a technique which is implemented to control one
pollutant can have various undesirable side effects,  such as promoting the
formation of another pollutant, degrading engine or vehicle performance, or
causing a  decrease in the effectiveness  of a remedial technique that is used to
eliminate  a different pollutant.
      Two appendixes are included. In Appendix 1, the spark-ignition
engine characteristics are briefly contrasted with those of compression-
ignition engines.  The differences discussed include the various operational
parameters, such as the means used  to control speed and power output, the
physical properties of the fuels used, the means used to introduce the fuel
into the combustion chambers, the means used to initiate the combustion
process, and the phenomena which  result in the emission of combustion
pollutants.
      Appendix 2 presents additional  information regarding hydrocarbon
molecular structure.  The discussion details the hydrocarbons present  in
gasoline fuels and the reconfigured and partially oxidized organic compounds
produced when some fuel molecules pass through the combustion chamber
of a spark-ignition engine without the complete liberation of the molecular
carbon atoms.

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Formation and Control of Combustion Pollutants
Blank page

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         Chapter 1. Gasoline-Fueled Spark-ignition Engines
      This synopsis focuses specifically on gasoline-powered, spark-ignition
engines.  Such engines utilize a throttled, spark-initiated, internal
combustion process to convert the chemical energy in the fuel into the
mechanical energy required for the operation of the motor vehicle.  This
conversion process takes place within several internal combustion chambers
similar to the one shown in Figure 1. The radial boundary of the chamber is
determined by the cylindrical cavity in the engine block. The engine head
provides the fixed end to the chamber.  The top of the reciprocating piston
provides the opposite movable end.  The combustible mixture of air and fuel
enters the combustion chamber via the inlet port and one or more intake
valves.  The combustion gases exit the combustion chamber via one or more
exhaust valves and the exhaust port.
Figure 1.  Engine Block and Head (cross-section)	
                             Spark Plug
                          Intake Valve
Exhaust Valve
     Head
                        Intake
                        Port
                 Cylinder
                  Combustion
                  Chamber
         Exhaust
         Port
           Head Gasket
                                                      Block
         Crank and Crankshaft
                                                         Flywheel
                                                     Connecting Rod

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Formation and Control of Combustion Pollutants
      As shown in Figure 2, the several inlet ports of the head are connected
to a common inlet by means of an intake manifold.  A throttle valve
regulates the ingestion of air or an air/fuel mixture, depending on the design
of the engine. The exhaust ports are connected to a common exhaust outlet
by means of an exhaust manifold.
Figure 2.  Engine Block and Manifolds.	
            Intake
            Manifold
             Inlet
             Throttle
             Valve
Exhaust Manifold
                                                         Outlet
      The four-stroke combustion cycle, which was first put to practical use
by Nicolaus A. Otto in 1876, is shown in Table 1 and Figure 3.  As Figure 3
illustrates, the four combustion phases do not start and stop at precise
positions of the piston, although they are affected by, or have  an effect on, the
four up-and-down strokes of the piston.
Table 1. Relationship of Combustion Phase and Piston Stroke.	
               Combustion Phase
        Air/fuel mixture is ingested
        Mixture is compressed
        Mixture is burned
        Combustion products  are expelled
  Piston  Stroke
  Intake
  Compression
  Power
  Exhaust
      This "Otto cycle" or spark-ignition process is both similar and different
from that of a compression-ignition process .  Appendix 1 provides a brief
contrast of the two types of engines and the resulting pollutants. This
synopsis focuses on pollutants formed by the combustion process in a
gasoline-powered, fuel-injected, four-stroke, spark-ignited motor vehicle
engine.

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                                           Gasoline-Fueled Spark-ignition Engine
Figure 3.  Spark-ignition Phases.
     Intake Valve
     Open

     Air/Fuel
     Mixture
                Both Valves
                Closed
         1) INTAKE STROKE
2) COMPRESSION STROKE
 Spark
 Initiated
 Flame
           POWER STROKE
                      Exhaust
                      Gas
                                           A) EXHAUST STROKE
      When a naturally aspirated (unturbocharged or unsupercharged)
spark-ignition engine is in operation, the movement of each piston away
from the cylinder head during the intake stroke increases the available space
in the cylinder. The increase in volume results in a decrease in pressure. The

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Formation and Control of Combustion Pollutants

accumulative effect of the successive intake strokes of the several pistons is
the reduction of the intake manifold pressure to a negative (subatmospheric)
value.  The extent to which the intake system pressure is reduced depends on
the speed of the engine and the position of the intake manifold throttle
valve.  The speed of the  engine in revolutions per minute determines the
total number of intake strokes per minute.  The position of the throttle valve
determines how much obstruction is offered to the inflow of ambient air.
The absolute pressure in  the intake manifold is the lowest (less than \
atmospheric pressure) at  idle and  highest (close to atmospheric pressure) at
wide open throttle.
      The subatmospheric pressure in the intake manifold facilitates  the
ingestion of ambient air via the air cleaner and the flow of the air to the
intake ports of the several cylinders via the individual passageways or
"runners"  in the intake manifold.  At some time prior to the arrival of the air
at each cylinder inlet port, "atomized" fuel in the form of very fine droplets is
added to the air. The fuel flow control system is designed to add the fuel at a
rate which will result in the  desired proportions of fuel and air.
      At each cylinder inlet port, the subatmospheric pressure in the
combustion chamber (which is lower than the subatmospheric pressure in
the intake manifold) facilitates the entrance of the air/fuel mixture. This
occurs when an intake valve opens as the piston moves away from the
cylinder head.  This is the first, or intake, stroke of the combustion cycle (see
Figure 3).
      The valve then closes and the piston moves toward the cylinder head
during the second, or compression, stroke. This movement compresses the
contained mixture and, as a consequence, heats it.  An electric spark ignites
the compressed and heated  air/fuel mixture sometime  during the time
interval when the piston is advancing toward and then retreating from "top
dead center" (the position where piston is at its closest point to the cylinder
head).
      The high pressure  developed as a result of this combustion process
forces the piston away from the cylinder head during the third (power) stroke
of the operating cycle.  The exhaust valve opens when the piston is again

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                                          Gasoline-Fueled Spark-ignition Engine

moving toward the cylinder head so that the combustion gases can be
expelled. This is the fourth and final (exhaust) stroke of the cycle.
      This sequence of events is repeated over and over in each cylinder of
the engine and  the combustion gases flow into the exhaust manifold and
escape into the  atmosphere via the vehicle tailpipe(s).  At any particular
moment, the  position of the air inlet throttle  valve determines the speed of
the engine and  the power it is developing. When the valve is in its "closed"
position, only enough air is ingested to allow engine operation at the desired
idle speed without the generation of any power for vehicle operation.  The
small amount of fuel added allows the generation of enough power to keep
the engine running smoothly at the  idle speed. When the throttle valve is
wide open and fuel is added at the appropriate rate, the engine is able to
develop its maximum power output. Then its speed is determined by  the
load requirements placed on it by the operation of the vehicle.
      If a hydrocarbon fuel containing no impurities could be burned  under
perfect conditions, the exhaust gases exiting the individual combustion
chambers would contain only:
      •  molecules of carbon dioxide (CO2) (containing the carbon atoms
         previously contained in the fuel molecules).
      •  molecules of water vapor (H20) (containing the hydrogen atoms
         previously contained in the fuel molecules).
      •  molecules of nitrogen (N2) (originally in the ingested air and not
         involved in the combustion process).
This can be represented by the following equation:
           Fuel (HC) + Air (O2 & N2) = Energy + CO2 + H2O + N2
      However, since most fuels contain some impurities and perfect
combustion conditions can not be realized in actual practice, the exhaust gases
may also contain varying percentages of:
      •  molecules of hydrogen (H2) which result when fuel hydrogen atoms
         are  not oxidized and associate to form diatomic molecules.
      •  fuel hydrocarbon (HC) molecules which were completely
         unchanged,  or only partially changed, during their passage through
         the  combustion chambers of the engine.
      •  molecules of carbon monoxide (CO) which are the result of the
         incomplete oxidation of the fuel carbon atoms.

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Formation and Control of Combustion Pollutants


      •  molecules of nitric oxide (NO) which were formed when the
         atmospheric nitrogen was subjected to the unique conditions
         existing in the engine's combustion chambers.
      •  molecules of inorganic compounds, such as sulfur oxides, which
         result from reactions involving fuel or lubricating oil impurities.

This can be represented by the following equation:

                       Fuel (HC) + Air (O2 & N2) =

             Energy + CO2 + H2O + N2 + H2 + HC + CO + NO

The formation and control of the pollutants resulting from these imperfect
combustion conditions are discussed in the following chapters of this
synopsis.
10

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         Chapter 2. Pollutant Formation — General Effects
      Two factors, fuel complexity and combustion complexity, have a
general effect on pollutant formation in that they preclude the complete
oxidation of the fuel.  Fuel complexity results from the many different kinds
of hydrocarbon compounds present in gasoline. Combustion complexity
results from the various structural and operational parameters of the engine
which affect the oxidation of these various compounds.
2.1. Fuel Complexity
      The term "gasoline" is used to describe the portion, or fraction, of
petroleum distillate which has a boiling point range of about 75 to 415°F. This
portion is a complex mixture of a wide variety of hydrocarbon compounds.
The molecules of all of these compounds are comprised of only two kinds of
atoms, carbon and hydrogen.  However, the  four attachment points at each
carbon atom allow an almost limitless variety of molecular configurations.
Some examples of these molecular structures are shown in Figure 4 and more
appear in Appendix Two.
Figure 4. Molecular Structure of Selected Hydrocarbons. _
                                       H-£-H H-C-H
          H   H   H  H             H    I   H   I    ?
          I1-!1-I*-I*-II       H-T-J'.-r   k—r   u
          i*   i*   i*  1*   n       "^+    *f   \*   i*    i*™""n
          M   U             * J.I»    i
                                          ri
              Butane                 Isooctane (2,2,4-trimethyl pentane)
      Gasoline hydrocarbons can be classified into three main types:
paraffins, olefins, and aromatics. The paraffin hydrocarbons are "saturated"
in that each molecule contains the maximum possible number  of
hydrocarbons atoms.  The olefin hydrocarbons are "unsaturated" or deficient
in hydrogen atoms as a result of double bonding between adjacent carbon
atoms in the chains. The aromatic hydrocarbons contain a unique structure,
known as a benzene ring, consisting of six carbon atoms in a closed chain or
                                                                    n

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Formation and Control of Combustion Pollutants

ring with single and double bonds alternating between the adjacent carbon
atoms. Each hydrocarbon class can be found in gasoline and in exhaust
emissions.  The actual percentage of each type of hydrocarbon depends on the
type of gasoline.
      The addition  of oxygen atoms to hydrocarbon molecules further
increases the number of possible molecular configurations.  In the case of the
alcohols, a hydrogen atom is replaced with a oxygen/hydrogen hydroxyl (-OH)
functional group. The two simplest alcohols, methanol (CHaOH) and ethanol
(CH3CH2OH), can be used alone as engine fuels or mixed with gasoline to
form oxygenated fuels. When aldehydes and ketones are formed during the
combustion of the fuel compound, a carbon atom is double bonded to one
oxygen atom in lieu of being single bonded to two hydrogen atoms.
      The physical properties of a hydrocarbon compound are affected by the
number of  carbon atoms in the molecule and the configuration of these
atoms within the molecular structure.  The effect of these details on physical
properties  is illustrated by Table 2.
      The first twelve compounds in Table 2 illustrate how an increase in the
number of  molecular carbon atoms results in an increase in boiling point and
a decrease in autoignition temperature. The decrease in the auto ignition
temperature results  from the increase in the susceptibility to thermal
breakdown which accompanies the increase in the length of the molecule.
      The last two compounds in the table illustrate how the configuration
of molecular carbon atoms affects  the boiling point and auto ignition
temperature.  The rearrangement of the six straight-chain carbon atoms in the
paraffinic hexane molecule into the aromatic benzene configuration results
in about a 14% increase in boiling point and about a 50% increase in auto
ignition temperature.  The rearrangement of the eight straight-chain carbon
atoms in the paraffinic octane molecule into the branched-chain isooctane
configuration (see Figure 4) results in about a 18% decrease in boiling point,
but about a 53%  increase in auto ignition temperature.
      Auto ignition temperature is one of the most important physical
properties of a gasoline hydrocarbon because it is an indication of detonation
tendency.  Detonation occurs when a portion of the air/fuel mixture in the
combustion chamber spontaneously ignites before the arrival of the spark-
12

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                                           Pollutant Formation—General Effects

induced flame front. Such detonation results in the generation of a second
very rapidly moving flame front.  The resultant rapid increase in pressure in
the combustion chamber produces the characteristic "knocking"  sound.
Table 2. Hydrocarbon Compounds and
Compound
Methane
Ethane
Propane
Butane
Pentane
Hexane
Heptane
Octane
Nonane
Decane
Undecane
Dodecane
Benzene
Isooctane3
Carbon
Atoms
1
2
3
4
5
6
7
8
9
10
11
12
6
8
Physical
State
Gas
ii
ii
ii
Liquid
ii
ii
11
it
11
11
Solid
Liquid
ii
Properties.
Boiling
Point
-259
-127
-44
31
97
155
209
258
303
345
384
4212
177
211

Auto
ignition
Temperature
1,346
1,050
995
961
933
909
893
880
871
866
—
—
1,363
1,350

Research
Octane
Number
no1
1041
100
92
61
25
0
-17
-45
—
—
—
110
100
  1 Estimated                 2 Melting point is 14°F      3 2,2,4-trimethyl pentane
      The octane number of a compound is an indication of its knocking
tendency, as can be seen in the preceding table. The use of such numbers
provides a means for rating the knocking,  or detonation, tendencies of
gasoline samples. This rating system is based on the knocking characteristics
of normal heptane (0 octane) and isooctane (2,2,4-trimethyl pentane) (100
octane) when a mixture of these hydrocarbons is burned in a Cooperative
Fuel Research single cylinder engine.
      The octane number of a gasoline sample indicates the relative amounts
(by volume) of isooctane and heptane in a mixture which exhibits a knocking
tendency comparable to that of the gasoline sample. For example, a gasoline
sample which has an octane rating of 80 has the same knocking tendency of a
mixture of 80% isooctane and 20% heptane. Fuel samples with a  lower
detonation tendency than isooctane are rated with a different rating scale.
This scale involves the supercharging of the test engine to increase the inlet
air pressure when isooctane is used as the  fuel.
                                                                      13

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Formation and Control of Combustion Pollutants

      By varying the operating conditions of the test engine, two different
values, the research octane number (RON) and the motor octane number
(MON), are obtained.  The RON value, the lower of the two, is obtained by the
use of more severe test engine operating conditions, such as a higher speed, a
more advanced ignition timing, and a higher intake mixture temperature in
the intake manifold.  The difference between the MON and RON values is
called the sensitivity of the sample. This value is used to indicate the
tendency of a fuel to preignite and produce knock  when the conditions under
which a vehicle engine is operating becomes more demanding.  The octane
value shown on the service station dispensing pump is the average of the
X,._XT    , 0~,.T   .    /MON + RON\
MON and RON values (	^	/•

      A typical gasoline sample will contain different  types of hydrocarbons
with molecular carbon atoms predominately in the C& to Ci2 range. The
carbon atoms in these  hydrocarbons can be, arranged in different
configurations.  (The tables in the appendix show a few hydrocarbon
molecular configurations in their simplest forms.)   A  specific gasoline
sample can also contain some hydrocarbons with fewer than six carbon
atoms. For example, some butane may be present, even though in the pure
state this hydrocarbon is a  gas at standard temperature and pressure
conditions. A gasoline sample may also contain hydrocarbon molecules with
more than 12 molecular carbon atoms, as well as configurations involving
various degrees of unsaturation and different combinations of straight and
branched chains and closed or aromatic rings.
      Since the composition of "gasoline" fuels can vary over such a wide
range, the combustion characteristics of a particular gasoline sample is
dependent on the nature of the contained mixture  of hydrocarbon
compounds. For this reason, EPA regulations specify  that emission testing
must be performed with gasoline which has properties that fall within
specified limits.  Furthermore, the test fuels must be either
      •  kept in sealed containers to prevent the preferential evaporation
         and escape of the hydrocarbons with the  lowest boiling points, or
      •  analyzed frequently enough to ensure that such preferential
         evaporation  or "weathering" does not result in changes which
         cause physical properties, such as octane  rating or vapor pressure, to
         exceed the specified tolerances.
14

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                                           Pollutant Formation—General Effects


2.2. Combustion Complexity

      The conditions and consequences of combusting or burning gas in the
open are different from those when gasoline is burned in the cylinders of a
spark-ignition motor vehicle engine.

      Burning in the open is a continuous process.  The surface of the liquid
fuel is exposed to atmospheric oxygen. When a flame is initiated, it is
maintained by
      1.  the continuous escape of hydrocarbon molecules from the liquid
         surface.
      2.  the heating of these molecules  to their kindling temperature.
      3.  the reaction of these molecules with oxygen (oxidation).

      Burning in an engine  cylinder is an intermittent or batch combustion
process which differs from an open burning process in that:
      1.  oxidation occurs with a specific quantity of fuel and air. Air is
         mixed with "atomized" fuel.  This mixture is not perfectly
         homogenous in that the size  and distribution of the liquid droplets
         is not completely uniform.
      2.  the air/fuel mixture is introduced into sealed combustion chambers
         which have complicated internal surfaces.  The mixture is then
         compressed and heated before it is ignited.
      3.  the combustion process in each separate combustion chamber is
         affected by numerous variables, such as:
         (a) the amount of change in air/fuel mixture uniformity, such as
            stratification which causes "top to bottom" variations in the
            distribution of the fuel droplets.
         (b) the amount of compression and, hence, the amount of heating
            the charge experiences prior to ignition.
         (c) the manner in which the spark-initiated flame front expands
            with the combustion chamber.
         (d) the degree to which the flame is extinguished as it approaches
            the relatively cool walls of the combustion chamber.
         (e) the amount of temperature and pressure rise that occurs during
            the combustion process.
         (f) the degree to which the limited time available for combustion
            affects  the completion of the process.

      An essential first step  in the oxidation of the gasoline hydrocarbon
compounds in the combustion chamber is the introduction of the air and fuel
                                                                      15

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Formation and Control of Combustion Pollutants

in the proper proportions. The appropriate ratio of air to fuel is determined
by:
      • the number of carbon atoms in the average fuel molecule, and
      • the ratio of hydrogen to carbon atoms in the average fuel molecule.
      If a fuel which has an average carbon atom chain length of six and the
average hydrogen atom/carbon  atom ratio of 1.86 is used, the chemically
correct or "stoichiometric" air/fuel ratio is 14.5 pounds of air to 1 pound of
fuel. Under perfect combustion conditions, the following results would be
obtained:
     14.5 Ib  air       =    1.07 lbO2  +  2.33 lbO2  +  11.1 Ib N2
     1.0 Ib  fuel      =    0.13  Ib H?  +  0.87 Ib C	
     15.5 Ib  exhaust  =   1.20 Ib H2O +  3.20 Ib CO2 +  11.1 Ib N2
      However, even when the  fuel is supplied at a rate that will
theoretically result in  chemically correct proportions of air and fuel,
optimum engine operation may  not be realized.  The desired results can be
precluded by a number of inhibiting factors inherent in the combustion
process. One of these factors is the change in the initial air/fuel ratio which
occurs before the mixture is actually introduced into the combustion
chamber.  The composition of this final mixture depends on a number of
details; such as, how well the fuel is "atomized," how well the fuel and air are
mixed, and how much exhaust remains in the combustion chamber to mix
with the incoming air and fuel.
      A second limitation is the incomplete utilization of the fuel that does
get into the combustion chamber.  As a consequence of these limitations,
engine operation for maximum  power output may require richer (less than
stoichiometric) ratios whereas operation for maximum fuel economy may
require  leaner (greater than stoichiometric) ratios.
      A number of factors can adversely affect the combustion process even
when the proportion of air to fuel is chemically correct. One of the most
important of these factors is the manner in which the air and fuel are
introduced into the combustion  chambers.  A perfect induction system
would:
16

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                                            Pollutant Formation—General Effects

       •  combine the fuel and air in a manner resulting in a perfectly
         homogeneous mixture of individual  hydrocarbon, oxygen, and
         nitrogen molecules, and
      •  deliver the mixture in a manner resulting in a perfect distribution
         between the individual  combustion chambers.
Such perfection is impossible, but an actual induction system should
minimize fuel droplet size, maximize the mixing of the droplets in the air,
and minimize adverse effects when the mixture is distributed between the
combustion chambers.  Carburetor-based fuel systems present limitations to
achieving this goal.
      When a carburetor-based system is naturally aspirated, subatmospheric
pressure  is used in two different ways. The downward movement of the
piston during the intake stroke results in a pressure drop in the intake
system. The decrease in pressure allows atmospheric pressure to force air into
the intake system via the air cleaner "and the associated runner of the intake
manifold. The flow of the incoming air through one or more venturi in the
carburetor results in another pressure drop which allows atmospheric
pressure  to force fuel into the air stream in the form of fine droplets. Such
use of atmospheric pressure for fuel induction places severe limitations on
the reduction of fuel droplet size and on the thorough mixing of these
droplets  with the incoming air.
      These particular limitations can be largely overcome by the use of an
injector which operates at a pressure in excess of atmospheric pressure and
sprays the fuel into the air stream. However, the use of such a  "throttle body"
injection  system does not eliminate adverse distribution effects. These
adverse effects can be caused by differences between the intake manifold's
individual runners or branches in regard to parameters such as temperature,
total length, and aerodynamic flow resistance.  Such differences can result in
the individual combustion chambers receiving air and fuel  in somewhat
different  proportions.  Such unequal distribution effects can be  minimized by
the use of a multipoint system in which a separate fuel injector is located in
the intake port of each combustion chamber.
      In  such multipoint systems, only the incoming air flows though the
throttle body and the intake manifold runners. Each individual injector is
operated by an electronic control unit in a manner which tends to result in
                                                                      17

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Formation and Control of Combustion Pollutants

the correct amount of fuel being delivered to the intake port of the associated
engine cylinder.  Some cylinder-to-cylinder differences in the air/fuel ratios
can result from distribution problems which can affect the flow of the air
through the runners of the intake manifold. Nevertheless, multipoint
injection systems largely eliminate the distribution problems that are
associated with single  point injection systems and carburetted systems.
      A number of engine configuration and timing details can affect the
combustion process. In regard to configuration details, some of the more
important factors are the locations of the spark plugs and the valves in the
chamber and the locations of the rings on the piston. In regard to timing
details, some of the most significant parameters are the opening and closing
of the intake and exhaust valves and the firing of the spark plugs. The
movement of the  intake and exhaust valves relative to the movement of the
piston  determines the  movement of the air/fuel mixture and the exhaust gas,
including the reverse flow of some of the exhaust gas when an "overlap"
condition results in the intake and exhaust valves being open at the same
time.  The timing of the spark generation determines when the ignition of
the air/fuel mixture is initiated  and, hence,  how much time is available for
the completion of the  combustion process.   The ignition timing therefore has
an effect on a number of variables such as the maximum pressure,  the mean
effective pressure, and the thermal efficiency.
      As a result of the unique conditions under which combustion occurs in
an internal combustion engine, fuel hydrocarbon molecules which  are not
completely changed by the oxidation process are partially altered  in various
ways.  Long chains can be severed and some of the resultant fragments can be
rejoined to form new molecular structures.  The new structures may have a
greater or lesser degree of unsaturation or ring formation than the original
compounds in the fuel. In addition, new compounds, such as aldehydes (see
Appendix 2), can be formed. Consequently, the proportion of a particular
class of hydrocarbons in the exhaust will be quite different to the  proportion
in the original gasoline fuel.  As a result of the reactions which occur in the
combustion chamber, the relative proportion of paraffinic and aromatic
compounds is reduced, the relative proportion of olefinic compounds is
increased, and new oxygenated organic compounds are formed.
18

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                                           Pollutant Formation—General Effects

      The use of a pure hydrocarbon compound, such as isooctane, as a fuel
in lieu of gasoline will reveal the effectiveness of the combustion process in
promoting complex chemical reactions. When the exhaust of an engine
using such a pure fuel is analyzed, hundreds of different hydrocarbon
molecules can be identified.  This complex variety reveals how extensively
the  original isooctane molecules were chemically altered during their passage
through the combustion chamber.
                                                                      19

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          Chapter 3. Pollutant Formation—Specific Effects

      In general, concern regarding the emission of combustion pollutants is
concentrated on three specific pollutants; i.e., hydrocarbons (HC), carbon
monoxide (CO), and nitric oxide (NO).  These three kinds of pollutants differ
in regard to the cause and effect phenomena which result in their presence in
the exhaust (see Table 3).

Table 3. Exhaust Pollutants.
     Pollutant Type            Cause                    Effect
          HC          Flame Quenching        Absence of fuel combustion
          CO          Inadequate oxygen   ,     Incomplete fuel oxidation
          NO          Excessive temperature     Nitrogen "fixation"
      As Table 3 indicates, HC emissions result  from portions of the air/fuel
mixture being partially or completely excluded from the combustion process.
The hydrocarbons in the exhaust are the residual fuel hydrocarbons which
passed through the combustion chamber without the oxidation of the
molecules.  Some of these fuel  hydrocarbons remain in their original form.
Some have their molecular structures changed as a result of the replacement
of hydrogen atoms by oxygen atoms or as a result of changes in the carbon
chain configuration. In all cases, the carbon  and hydrogen atoms remain
bound  in some hydrocarbon or oxygenated organic molecular structure and
are not fully oxidized to carbon  dioxide (COz) and water (HiO).
      When fuel hydrocarbon molecules completely react with the oxygen
molecules during the combustion process,  the carbon atoms are oxidized to
carbon dioxide (COz) and the hydrocarbon atoms are oxidized to water vapor.
However,  a small fraction of the fuel molecules  undergo less complete
conversions and different results are obtained. The carbon atoms are only
partially oxidized to carbon monoxide (CO).  Instead of hydrogen atoms being
oxidized, they associate with each other  to form diatomic hydrogen
molecules.
      NO emissions are unique relative to CO and HC emissions in that NO
formation is not directly related to the combustion process. The oxidation or
"fixation" of the atmospheric nitrogen would occur without the presence of
any hydrocarbon fuel.  At the high temperatures which occur in the
combustion chamber, a fraction of the atmospheric nitrogen and oxygen
                                                                     20

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                                           Pollutant Formation—Specific Effects

molecules react to form NO molecules which are subsequently converted to
other nitrogen oxides, such as nitrogen dioxide (NO2).
      Details regarding the three phenomena causing each of these
conditions are presented in the following sections.
3.1. Effect of Flame Quenching on HC Emissions
      When a gasoline-fueled spark-ignition engine operates under
favorable conditions; i.e., close to a stoichiometric air/fuel ratio and with an
absence of malfunctions such as ignition misfire, the primary source of
hydrocarbons in the exhaust is the fuel molecules which were not adequately
involved in the combustion process.  Some of these molecules may have
undergone some structural changes, such as a reduction in carbon-chain
length or a replacement of some of the hydrogen atoms by oxygen atoms.  The
remainder of the uninvolved molecules will have passed unchanged
through the combustion chamber as~a consequence of being isolated from the
combustion process as a result of "flame quenching."
      When a flame in the combustion chamber is initiated at the spark plug,
it expands very rapidly in all directions.  However, quenching, or extinction,
due to heat transfer can occur at the boundaries of the expanding "ball" of
flame.
      Wall quenching occurs when the flame front approaches the physical
boundaries of the combustion chamber where a sharp drop in temperature
occurs (see Figure 5).  The fuel in close contact with these boundaries has a
lower temperature as a result of its proximity to  the cooler metal surfaces.
When the temperature is too low to support combustion, the flame is
quenched.

Figure 5.  Flame Quenching.	
                                      ^—Wall Quenching

                                          Crevis Quenching
                   Rame Front
                                                                      21

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Formation and Control of Combustion Pollutants

      Restriction, or crevis, quenching occurs when the flame front reaches a
restriction which impedes further propagation.  Typically, the flame
encounters such a restriction when it reaches any very small volume in the
combustion chamber.  One such flame quenching volume is the cavity that is
formed by (a) the upper surface of the topmost piston ring, (b) the outside
diameter of the piston, and (c) the inside diameter of the cylinder (see Figure
5).
      Regardless of the cause, when the flame is quenched, the fuel in the
volume  beyond the boundary where quenching occurs is more or less isolated
from the combustion process. One fraction of this isolated fuel leaves the
combustion chamber essentially in its original unaltered state.  Another
fraction leaves in an altered state, as a result of low temperature preflame
reactions in the quenched zones.  These altered molecules appear in the
exhaust in form of aldehydes and other partially oxidized compounds (see
Appendix 2. Oxygenated Organic Compounds.).
3.2. Effect of Oxygen Content on CO Formation
      As was previously mentioned, some fuel hydrocarbon molecules do
not completely react with oxygen molecules during the combustion process
and the  carbon atoms are only partially oxidized to carbon monoxide. The
likelihood of such results occurring decreases as the availability of oxygen
increases. However, even when relative proportions of oxygen and fuel
molecules are considerably in excess of the stoichiometric, or "chemically
correct"  proportion,  a very small fraction of the fuel carbon atoms are still
only partially oxidized  to carbon monoxide molecules.
3.3. Effect of Temperature on NO Formation
      Unlike HC and CO emissions, NO emissions do not arise as a
consequence of the incomplete oxidation of the fuel.  NO emissions result
from a side reaction that occurs under the unique conditions produced in the
combustion chamber when the fuel is oxidized. These conditions are quite
different than those that prevail when gasoline is burned in the open.
      During open burning conditions, the nitrogen molecules in the air  are
not affected by the combustion process and atmospheric nitrogen acts as a
non-reactive diluent. However, when gasoline is burned in the cylinders of
an internal combustion engine, the high temperatures and pressures that  are
22

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                                           Pollutant Formation—Specific Effects

produced cause some "fixing" of atmospheric nitrogen. A small percentage of
the nitrogen molecules are "fixed" when they combine with oxygen in the
combustion chamber. The primary immediate reaction product is nitric oxide
(NO) which can undergo conversion into other oxides, such as nitrogen
dioxide (NO2), during transit through the exhaust system or during
subsequent dispersion into the atmosphere.
                                                                      23

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              Chapter 4.  Pollutant Control Approaches
      Two general approaches for minimizing the emission of pollutants
from the tailpipe of a motor vehicle may be taken:
      •  the preventive approach which involves the modification of the
         combustion conditions  to minimize the formation of pollutants in
         the combustion chamber, and
      •  the remedial approach which involves the treatment of the exhaust
         gas to minimize the concentrations of the pollutants which exit the
         combustion chamber.
Each approach uses a variety of techniques. This chapter discusses each of
these techniques and the possible interactions and complications of these
techniques.
4.1. Preventive Techniques
      The three specific preventive techniques are
      •  changes in engine design (combustion chamber redesign),
      •  changes in engine operation (fuel flow controls), and
      •  changes in combustion conditions (temperature reduction).
These techniques will affect hydrocarbon, carbon monoxide, and nitric oxide
emissions, respectively.
4.1.1. Combustion Chamber Redesign for HC Minimization
      Flame quenching results in some fuel hydrocarbon molecules exiting
unaltered, or partially altered, from the combustion chamber (see Chapter 3).
Combustion chamber redesigns can minimize the effects of this
phenomenon. Quenching due to wall effects can be reduced by design
changes that reduce the surface area  of the combustion chamber relative to
the clearance volume (piston is at top dead center). Combustion chamber
design changes that can be implemented to accomplish the desired decrease in
the surface to volume (s/v) ratio  include:
      •  reducing depressions and protrusions in the chamber.
      •  changing the nature of the  surfaces that provide the clearance
         volume (see Figure 6).
      •  making the cylinder geometry more favorable.
                                                                     24

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                                                 Pollutant Control Approaches
      Restriction quenching can be reduced by any chamber redesign which
eliminates or reduces any small volume that impedes the propagation of the
flame front.  For example, if the topmost piston ring is moved up toward the
end of the piston (see Figure 1), a volume reduction is realized in the annular
cavity which is formed around the top of the piston.  Consequently, the
amount of fuel which is isolated from the oxidation process is reduced.
Figure 6.  Surface/Volume  Ratio Changes.	
                   Combustion Chamber Shape Changes
              Cylinder,,
               Head
                Piston •
                S/V
8.0
7.2
6.6
6.4
4.1.2. Fuel Control for CO Minimization
      As was mentioned in section "3.2. Effect of Oxygen Content on CO
Formation," an increase in the availability of oxygen tends to decrease the
number of fuel carbon atoms that are only partially oxidized to carbon
monoxide.  Such increase in oxygen availability can be accomplished by
reducing fuel input to increase the air-fuel ratio beyond the stoichiometric
ratio so that combustion occurs under lean conditions.
      However, such a lean approach to minimization of carbon monoxide
formation is limited by several possible undesirable side effects, such as rough
engine operation, increased nitrogen oxide formation, and adverse effects on
downstream exhaust aftertreatment devices.  Moreover, beyond a specific
ultimate limit in lean operation, the proportion of fuel molecules to oxygen
molecules becomes too low for efficient combustion. At that point, the
mixture of  air and fuel fails to ignite and "lean misfire" occurs.
4.1.3. Temperature Control for NO Minimization (Exhaust Gas Recirculation)
      Fixing atmospheric  nitrogen within the combustion chamber can be
inhibited by any mechanism that reduces the maximum temperature
developed  during  the combustion process. As was previously mentioned,
one means for accomplishing the necessary temperature reduction is
                                                                      25

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Formation and Control of Combustion Pollutants

retarding the spark. This change reduces the maximum temperature by
shortening the time available for the completion of the combustion process.
However, retarding ignition has disadvantages, such as the loss of power
output that results from the  reduction in the maximum pressure in the
cylinder.
      A more satisfactory means of lowering the maximum combustion
temperature is to increase the heat capacity of the gases in the combustion
chamber by diluting the new charge of air/fuel mixture with a gas that does
not take part in the combustion process.  The exhaust gas is ideally suited for
this purpose because:
       • it is readily available and  can be easily recirculated back into the
         combustion  chamber.
      •  it has a high concentration of carbon dioxide and water molecules
         which have  higher heat absorption capacities than the molecules of
         a diatomic gas, such as atmospheric  nitrogen.
      Some dilution of the new mixture charge by exhaust gas is inherent in
the four-stroke combustion cycle. At the completion of the exhaust stoke,
some of the exhaust gas, which is at a pressure in excess of atmospheric
pressure, is left behind in the clearance volume which remains when the
piston is top dead center. When the intake valve opens at the start of the
intake stroke and exposes the cylinder to the subatmospheric pressure in the
intake system, pressure equalization occurs.  As a result, a fraction of the
residual exhaust backflows through the open intake valve and mixes with,
and dilutes, the entering new charge of air/fuel mixture.  Further dilution of
the mixture is caused by the fraction of the exhaust which did not back flow
out through the intake valve  and remained in the cylinder.
      Such inherent dilution  is  considerably enhanced when there is a
"valve overlap" condition in which the exhaust valve is  still open when the
intake valve opens (see Figure 7).  The reduction in cylinder pressure which
results from the downward movement of the  piston during the intake stroke
results in a fraction of the exhaust gas which was forced out of  the
combustion chamber into the exhaust port during the exhaust  stroke
reentering the cylinder via the open exhaust valve.  The primary purpose of
such valve overlap is  to produce the desired engine performance
characteristics.  Nevertheless, the resultant recirculation of exhaust gas results
26

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                                                Pollutant Control Approaches

in some reduction in the maximum combustion temperature and, hence,
some reduction in NO formation.

Figure 7.  Internal Exhaust Gas Recirculation (Valve Overlap).	
               Air/Fuel mixture
                                           Both valves open
                                                Exhaust
      When such inherent exhaust gas recirculation does not provide the
desired reduction in NO formation, additional exhaust gas flow must be
provided by means of some routing external to the combustion chamber.
Such an "add-on" exhaust gas recirculation (EGR) emission control system
can consist of (a) a connecting passageway between the intake and exhaust
manifolds of the engine and (b) a valve which controls the flow of exhaust
gas through the passageway (see Figure 8).  The EGR system control
mechanism is designed to open and close the valve as needed to minimize
the formation of NO while also minimizing any undesirable effects on
performance characteristics, such as a poor idle quality or reduced
performance during wide open throttle acceleration.
4.2. Remedial Techniques
      Two techniques are used remedially to remove pollutants which exit
the combustion chamber:
      •  thermal oxidation in the exhaust manifold
      •  catalytic conversion in the exhaust stream
The first of these techniques uses supplemental air to oxidize HC and CO
pollutants. The second oxidizes HC and CO and reduces NO pollutants.
4.2.1. Supplementary Air Oxidation
      As discussed  previously under preventive techniques, operating an
engine under very lean conditions can reduce CO but a number of factors
                                                                     27

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Formation and Control of Combustion Pollutants

preclude such operation. However, atmospheric oxygen can be added to the
exhaust stream after the exhaust gases leave the combustion chamber. Such
oxygen enrichment facilitates the continuation of the oxidation reactions that
were initiated in the combustion chamber.  The secondary air is injected
directly into the exhaust ports of the cylinders.  The carbon monoxide and
hydrocarbons in the very hot exhaust  gases are thermally oxidized without
the production of a  visible flame.  One side benefit of such secondary air
injection during cold starting is that the increase in exhaust gas temperature
occurring as a result of the oxidation reactions reduces the time required for
the downstream catalytic converter to reach the temperature necessary for
efficient oxidation conversion.
Figure 8.  External Exhaust Gas Recirculation.	
            Intake
            Manifold
Exhaust Manifold
                                     Control Signal
      Depending on the purpose for the introduction of additional air into
the system, negative or positive pressures (below or above atmospheric
pressure) can be used to provide the necessary differential pressure. For
example, a negative pressure system can be used when the purpose of
secondary air introduction is to reduce emissions during idle operation,
particularly when a cold engine is started and is warming up. During such
engine operation, the concentration of oxygen in the exhaust manifold is too
low to effectively oxidize the CO and HC in the exhaust gas.  The necessary
additional oxygen can be introduced by means of a simple aspiration system
28

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                                                  Pollutant Control Approaches

which takes advantage of the negative pressure pulses in the exhaust
manifold.
      In the simplest form of such a system, the necessary air flow control
functions are performed by a one-way aspirator valve located in a line
connecting the exhaust port air injection tubes with an inlet for atmospheric
air, usually in the air cleaner (see Figure 9).  The aspirator valve allows the
entrance of atmospheric air, but prevents the escape of exhaust  gas. When
the engine is idling and a large negative (below atmospheric) pressure pulse is
produced at an exhaust port as the result of the opening of the associated
exhaust valve, the higher atmospheric  pressure forces the aspirator valve
open. Atmospheric air flows into the system and exits at the exhaust port via
the air injection tube. As soon as the exhaust valve closes and the pressure at
the exhaust port rises above atmospheric pressure, the higher pressure closes
the aspirator valve and the escape of exhaust gases into the atmosphere  is
prevented.

Figure 9.  Aspirated Air Injection.	
         Intake
         Manifold
Exhaust Manifold
      Air
      Cleaner
                         Aspiration valve
      In some systems, secondary air is injected into the exhaust ports to
promote thermal oxidation reactions and into the exhaust system,
downstream of a three-way catalyst but upstream of an oxidation catalyst, to
promote catalytic oxidation reactions. In such systems a positive pressure
                                                                        29

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Formation and Control of Combustion Pollutants
system must be used.  The required higher than atmospheric pressures are
provided by an engine-driven mechanical air pump (see Figure 10). When
the engine warmup process has been completed, the output of the pump is
switched from the exhaust manifold to the  injection point in the exhaust
system upstream of the oxidation catalyst. The added air ensures that
sufficient oxygen is in the converter for the required conversion efficiency.
Figure 10.    Forced Air Injection.	
        Intake
        Manifold
                               Exhaust Manifold
     Air
          Filter
Air Pump
Diverter
Valve


J
Three-way
Catalyst
                                                            Oxidation
                                                            Catalyst
4.2.2. Catalytic Conversion
      Another aftertreatment of the exhaust gases, catalytic conversion,
involves promoting chemical reactions which involve the CO, HC, and NO
emissions. These polluting forms of carbon and nitrogen are then changed
into non-polluting forms. The use of such exhaust aftertreatment as a
remedial pollution control is made possible by catalytic converters which
have the required performance characteristics.  Such converters must be  able
to selectively promote the chemical reactions producing the desired results
30

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                                                 Pollutant Control Approaches

and to suppress other possible competitive reactions which either lower
effectiveness or yield undesirable by-products.
      Chemical Reactions—The carbon atoms in the combustion gases are in a
polluting form when they exist in CO and HC molecules.  If sufficient oxygen
is present, passage through a "two-way" oxidation catalytic converter will
result in a significant fraction of the CO molecules being oxidized to CO2
molecules and the HC molecules being oxidized to COz and water (H2O)
molecules .
      The nitrogen atoms in the combustion gases are in a polluting  form
when they exist as nitric oxide (NO) molecules.  When sufficient reducing
agents are present, passage through a reducing catalyst will result in a
significant fraction of the nitric oxide molecules being reduced to atmospheric
diatomic nitrogen molecules (N2).
      The desired reactions, the oxidation of CO and HC and the reduction of
NO, can occur more or less simultaneously when the exhaust gas is passed
through a "three-way" oxidizing/reducing converter if the upstream
composition of the exhaust is appropriately controlled. Such control of
exhaust gas composition is necessary because the reduction of the NO to
diatomic nitrogen (N2) is somewhat more complex than the oxidation of CO
and HC to CO2 and H2O.
      In the oxidation conversions, new molecules are formed  when their
precursor "raw material" component parts combine with  each other.
However, the reverse does not occur in connection with the NO reduction.
The process is not as simple as the breakup of the NO molecules with the
release of both the nitrogen and oxygen atoms back to the atmosphere. The
reduction of NO depends on the  interaction of NO with other exhaust
reducing components in various  reactions, such as the following:
            2NO + 2H2     =   N2 + 2H2O
            2NO + 2CO    =  N2 + 2CO2
            4NO + CIV   =   2N2 + CO2 + 2H2O
      In connection with the above reactions, the following facts are worth
noting:
1 Where the methane molecule, CH4, represents all possible HC molecules.
                                                                      31

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Formation and Control of Combustion Pollutants

      •  all of the NO reduction conversions depend on the presence of
         reducing agents, such as H2, CO, and HC.
      •  the last two reactions result in the elimination of all three
         pollutants, NO, CO, and HC.
      System Requirements—The actual hardware that can be used to accomplish
the desired conversion reactions depends on the requirements of a particular
system. For example:
      •  if NO emissions are  not a problem, a two-way oxidizing converter
         can be used to oxidize CO and HC,
      •  when NO emissions  are a problem, a three-way catalyst can be used
         to simultaneously reduce NO and oxidize CO and HC, or
      •  if a three-way catalyst alone does not adequately lower the
         concentrations of CO and HC,  a downstream oxidizing catalyst (see
         Figure 10) can be added to further lower the concentrations of these
         pollutants.2
      The performance of catalytic converters is affected by the chemical
composition of the exhaust.  In the case of oxidizing converters, the
relationship between composition and performance is fairly straight-forward.
When the oxygen concentration falls to a level which inhibits the oxidation .
of CO and HC, performance is  degraded.
      In regard to three-way converter operation, the relationship between
composition and performance is more complex .  Such a  converter will yield
the desired results only when  the concentrations of all of the several reactants
remain within a limited range. For example, if the concentration of oxygen
remains too low relative to the concentrations of CO and HC (as a result of
continuous engine operation under rich conditions), adequate oxidation
conversion of these pollutants will not be possible. Similarly, if the
concentrations of reducing agents, such CO and HC, remain too low relative
to the concentration of NO (as a result of continuous engine operation under
lean conditions), adequate reduction conversion of NO will not be possible.
The solution to the problem which results from  these conflicting
requirements is to rapidly oscillate the exhaust composition between slightly
2 The three-way catalyst and the oxidizing catalyst can be housed in one container or they can
  be housed in two separate containers. If necessary, air can be injected upstream of the
  oxidizing catalyst to ensure an adequate concentration of oxygen in the oxidizing catalyst.
32

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                                                  Pollutant Control Approaches

lean (slight excess of oxygen) and slightly rich (slight excess of reducing
agents) conditions.
      Since exhaust composition depends on the composition of the ingested
mixture or the air/fuel ratio, the possibility exists of using exhaust gas
composition information to regulate fuel introduction.  Regulating fuel
introduction can then maintain the air/fuel ratio within the range that
maximizes engine and converter performance.  The operation of such a
closed loop "feedback" fuel control system involves:
      1. generating some output signal that is dependent on the exhaust gas
         composition.
      2. detecting any change in that signal indicating that the air/fuel ratio
         needs to be adjusted.
      3. adjusting the fuel flow rate to result in the desired air/fuel ratio.
The successful operation of such a system is dependent on its ability to make
effective use of the small changes in exhaust composition which occur when
air/fuel ratio deviations are held within the desirable narrow tolerance band.
      The concentrations of all of the exhaust components, such as HC,  CO,
NOX, and 02, undergo very gradual changes when the air/fuel ratio varies
over a very wide range. This effect is illustrated in the following table of
typical oxygen (02) and carbon monoxide (CO)  concentrations when the
stoichiometric (chemically correct) ratio for a specific fuel is 14.7.
Table 4.   O2 & CO Concentration by Air/Fuel Ratio.
Air/Fuel Ratio
(Lbs. air/lb. fuel)
13.9 (very rich)
14.6 (rich)
14.7 (stoichiometric)
14.8 (lean)
15.3 (very lean)
02
(Volume %)
0.3
0.5
0.6
0.7
1.2
CO
(Volume %)
1.4
0.4
0.3
0.2
0.1
As this table indicates:
      •  the changes in O2 and CO concentrations are very gradual when the
         air/fuel ratio varies over a wide range from very rich (excess fuel) to
         very lean (excess air) or vice versa.
      •  the changes in O2 and CO concentrations are very slight when the
         air/fuel ratio deviates slightly from the stoichiometric ratio.
                                                                       33

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Formation and Control of Combustion Pollutants

       •  when the air/fuel ratio is very rich (13.9), the concentration of Oz is
         still about one half of the C>2 concentration when the air/fuel ratio is
         stoichiometric.
       •  when the air/fuel ratio is very lean (15.3), the CO concentration is
         still about one third of the CO concentration when the air/fuel ratio
         is stoichiometric.
       A fuel control system that is dependent on such small changes in the
concentration of a particular exhaust gas component would have to meet or
exceed very demanding performance criteria in regard to:
       •  the amount of air/fuel ratio deviation occurring before the need for
         a change in fuel flow rate is indicated, and
       •  the time delay between the fuel flow rate change and the
         elimination of the excessive air/fuel ratio deviation.
       Such system requirements would be much more demanding under the
non-steady state conditions that typify the .operation of motor vehicle
engines.  During the operation of such engines, fuel flow requirements are
greatly complicated by the numerous and rapid changes in engine speed and
load that occur.
       A more promising approach is to make use of the relative changes in
the exhaust gas components. As Figure  11 shows, the  concentration of oxygen
decreases and the concentrations of reducing agents, such as hydrogen and
CO, increase as the composition of the exhaust changes from slightly lean to
slightly rich. The exhaust gas parameter which would have to be monitored
would be the shift in the lambda of the exhaust, from rich (lambda < 1) to
lean (lambda > 1), or vice versa, relative to the stoichiometric value.3
Closed  Loop Fuel Control System—Such a "stoichiometric shift" approach to exhaust
composition control is utilized in the closed loop fuel  control system that is
pictured in Figure 12.  As is shown, the lambda sensor is installed upstream of
the three-way catalyst to provide a signal which is used by the electronic
control module (ECM). Depending on the "feedback"  signal which is
generated by the lambda sensor, the ECM makes the changes in the fuel flow
  A "lambda" value indicates how the actual proportions of oxygen and reducing agents in an
  exhaust gas mixture compare with the chemically correct or stoichiometric proportions that
  would be necessary for the complete reacttion of the oxygen with the reducing agents.
  Lambda is less than one when the exhaust composition is less than stoichiometric (rich
  conditions with excessive reducing agents) and more than one wihen the exhaust composition
  is greater than stoichiometric (lean conditions with excessive oxygen).
34

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                                                 Pollutant Control Approaches
rate necessary to keep the exhaust composition close to stoichiometric.  The
control "loop" is "closed" when the sensor reacts to the change in exhaust gas
composition resulting from the change in the fuel flow rate.

Figure 11.   Exhaust Composition.                ~~~
 O
 W
 O
     0.5
                                                                     _% CO
      .%H2

      .% HC
       0.97
1.03
      The detecting element of the lambda sensor is a tetravalent zirconium
oxide (ZrO4) ceramic thimble. This thimble is installed in the exhaust pipe so
that the interior of the thimble is in contact with the outside atmosphere and
the exterior is exposed to the exhaust gases. The zirconium oxide thimble is
impermeable to atmospheric oxygen or any gas which is in atomic or
molecular form.  However, a very small amount of a lower valent oxide,
such as the trivalent yttrium oxide (Y2O^), is dispersed in the zirconium
oxide.  The yttrium oxide provides anion vacancies which allow oxygen ions
(with two negative charges) to diffuse through the walls of the thimble.
Portions of the interior and exterior of the thimble are covered with porous
platinum coatings which function as conductive electrodes and as catalyzing
surfaces.
                                                                      35

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Formation and Control of Combustion Pollutants
Figure 12.   Closed Loop Fuel Flow Control System.
AIR
                       ENGINE
  FUEL-
                                     LAMBDA SENSOR
                                                       3 WAY CATALYST
                       INJECTION
                           FUEL
                           QUANTITY
                           SIGNAL
        AIR
        QUANTITY
        'SIGNAL""
ELECTRONIC
 CONTROL
   UNIT
                                                                  EXHAUST
                                                                  GAS
                                  LAMBDA SIGNAL
      In this application, the lambda sensor functions as a voltaic cell which
generates a signal voltage. This voltage is generated when the oxygen which
migrates through the sensor thimble reacts with reducing agents, primarily
hydrogen and carbon monoxide, in the exhaust.  When the air/fuel mixture
ingested by the engine is lean, the exhaust contains more oxygen than
necessary for reaction with the reducing agents present. Under these
conditions, very little opportunity exists for the reaction of the reducing
agents with the oxygen migrating through the sensor thimble and the output
voltage remains at about 0.1 volt.
      When the air/fuel mixture is rich, the exhaust contains less oxygen
than needed for the reaction with the reducing agents.  Under these
conditions, the reducing agents can react with oxygen which migrates
through the sensor thimble  and  a voltage potential of about 0.9 volts is
developed. The switch-like operation of the lambda sensor is illustrated in
Figure 13.
      In the closed loop fuel flow control system shown in Figure 12, the
air/fuel ratio continuously oscillates between conditions that are slightly rich
or lean relative to the stoichiometric value.  By optimizing the system, both
the magnitude of the deviations of the  air/fuel ratio from the stoichiometric
36

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                                                 Pollutant Control Approaches

value and the duration of the deviations can be reduced.  Such optimization
reduces HC and CO tailpipe emissions by
      •  reducing the emission of the pollutants from the individual
         combustion chambers as a result of the operation of the engine with
         an air/fuel ratio close to stoichiometric, and
      •  reducing the concentrations of the pollutants in the exhaust stream
         as a result of the operation of the catalytic converter at the
         maximum effectiveness which results when  the concentrations of
         oxygen and reducing agents in the exhaust are held close to their
         stoichiometric values.

Figure 13.   Lambda Sensor Operation.
    800
 ~
 .1  600
 HI
 o
 §
 cc
 I
 tu
400
300
    100
      0.97
            0.98
0.99
1.01
1.02
1.03
                                 LAMBDA
4.3. Interaction Complications
      The application of the preceding control techniques is greatly
complicated by the complex interactions that these techniques have on each
other.  The use of one technique to accomplish a specific change, such as the
reduction of one type of pollutant, may result in another change which
produces an undesirable effect.  For example, a change in engine operating
conditions which reduces the formation of one type of pollutant can increase
                                                                      37

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Formation and Control of Combustion Pollutants

the formation of another type of pollutant.  The change in engine operation
may also have other undesirable affects, such a degradation of performance,
an increase in  fuel consumption, or an exhaust temperature decrease which
may have an adverse effect on a downstream aftertreatment device.
      This tendency of an engine operating change to simultaneously
produce desirable and undesirable results is particularly troublesome in
regard to the hydrocarbons and nitric oxides in the exhaust. This dilemma
results from the fact that an increase in combustion efficiency tends to
decrease exhaust hydrocarbons but increase exhaust nitric oxides. The
increase in combustion efficiency results in a more complete oxidation of the
fuel and, hence, a decrease in exhaust hydrocarbons. However, the increase
in combustion efficiency results in an increase in the maximum temperature
in the combustion chamber and, hence, an increase in exhaust nitric  oxide as
a consequence of the increase in the fixation of atmospheric nitrogen.
Changes which decrease combustion efficiency and, hence, decrease nitric
oxide formation, such as rich engine operation (excess fuel) and spark
retardation, tend to increase the concentration of hydrocarbons in the exhaust
and decrease engine efficiency  and fuel economy.  In these situations, a
compromise is made to provide a balance between positive and negative
effects.
38

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Appendixes
                   39

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 Formation and Control of Combustion Pollutants
40

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                             Appendix 1.
                     Comparison of Four-Stroke
          Spark-ignition and Compression-ignition Engines

      Four-stroke spark-ignition and compression-ignition engines are
similar in that they:
      •  use an intermittent internal combustion process in which the high
         pressure combustion gases are directly used as the working fluid.
       •  (External combustion engines, such as steam engines, use a
         continuous combustion process to heat a separate working fluid.),
      •  burn liquid hydrocarbon fuels,
      •  incorporate reciprocating pistons, and
      •  use four piston strokes to complete each combustion cycle.
      However, these two types of engines differ in regard to:
      •  the means by which engine speed and power output are controlled,
      •  the physical properties and combustion characteristics of the
         required fuels,
      •  the manner in which the fuel is  introduced into the combustion
         chamber,
      •  the technique which is used to initiate the combustion process, and
      •  the mechanisms which result in the formation of combustion
         pollutants.
      The significance of  these differences between the two types of engines
are briefly discussed in the following paragraphs. This discussion  excludes
engines which use superchargers or turbochargers to blow air into the engine
intake systems. Furthermore, the discussion excludes two-stroke cycle
engines.  At the present time, two-stroke, gasoline-fueled, spark-ignition
engines are not used to power light-duty motor vehicles and only one engine
manufacturer produces two-stroke, diesel-fueled, compression ignition
engines for use in heavy-duty vehicles.
Speed and Power Output  Control
      In  spark-ignition engines, air flow is the primary control parameter.
The accelerator is connected to  a throttle valve which regulates the rate at
which atmospheric air enters the intake system. Prior to the flow  of the air
into each combustion chamber, fuel is added in an amount resulting in an
                                                                     41

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Formation and Control of Combustion Pollutants

air/fuel mixture which will produce the desired engine speed and power
output.
      In compression-ignition engines, fuel flow is the primary control
parameter. The accelerator is connected to fuel injectors which inject into
each combustion chamber subsequent to the ingestion of the intake air, the
amount of fuel needed for the desired engine speed and load. The entrance of
atmospheric air into the engine intake system is uncontrolled.  Consequently,
when the engine is not operating at maximum speed and power output, the
amount of air ingested is in excess of that needed for the complete
combustion of the fuel.
Fuel Properties
      In spark-ignition engines, the required gasoline fuels are comprised of
complex mixtures of hydrocarbon compounds.  These mixtures have
distillation ranges of about 75 to 415°F. The majority of the hydrocarbon
molecules in these mixtures have carbon atom numbers that range from six
to twelve  in number.
      The preignition ("detonation") or knocking tendency of a gasoline fuel
is indicated by an octane number.  In this rating system, normal heptane (Cy)
has an octane number of 0 and isooctane (Cg) (2,2,4-trimethyl pentane) has an
octane number of 100. An octane number close to 90 is normally adequate for
an engine which does not require a premium grade fuel.
      In compression-ignition engines, the required diesel fuels are
comprised of mixtures of hydrocarbons with distillation ranges of about 340 to
about 660°F. The majority of the hydrocarbon molecules have carbon atom
numbers that range from about Cu to QS.
      The spontaneous ignition characteristic of a diesel fuel is indicated by
its cetane number. In this rating system, heptane (€7) has a cetane number of
57 and hexadecane, or "cetane" (Qe), has a cetane number of 100.  A cetane
number in the 40 to 50 range is usually adequate.
Fuel Introduction
      In spark-ignition engines, "atomized" fuel in the form of minute
droplets is added to the incoming air by means of a carburetor or one or more
low pressure injectors.  Atmospheric pressure forces the resulting mixture
42

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                                                            Appendix One

into each combustion chamber during the intake stroke of the cycle. The
mixture is subsequently compressed during the compression stroke.
      In compression-ignition engines, fuel is injected into each combustion
chamber (or prechamber) after the air has been ingested during the intake
stroke of the cycle and then compressed during the compression stroke. The
fuel is introduced into the chamber in the form of a spray of very small
droplets. This spray results from the use of injectors, operating at pressures of
several thousands of pounds per square inch, to force the fuel through very
small openings in the injector tips.
Combustion Initiation
      In spark-ignition engines, the ingested air/fuel mixture undergoes a
compression of about 8 to 1 during the compression stroke of the cycle. As a
consequence, pressures of 120 to 400 pounds per square inch and temperatures
of around 900  °F are developed in the combustion chambers.  The increase in
temperature is not great enough to cause the spontaneous ignition of the fuel.
Therefore, the  combustion of the air/fuel mixture is initiated by means of an
electric spark generated between the electrodes of one or more spark plugs.
The flame then expands to fill the combustion chamber as the fuel in the
mixture is progressively oxidized.
      In compression-ignition engines, the ingested air undergoes a
compression of about 15 to 1.  As a consequence, the pressure of the air is
increased to about 400 to 800 pounds per square inch and its temperature is
increased to about 1400°F. At such elevated air temperatures, the fuel
undergoes spontaneous ignition almost as soon as it emerges from the holes
in the injector  tips.
Pollutant Formation
      In spark-ignition engines, pollutant formation problems include (a) the
fuel wetting of the walls of the intake system, (b) the introduction of rich
mixtures into the combustion chamber, and (c)  the quenching of the flame
after it is initiated.  Two different phases of the combustion process can affect
pollutant formation.  The first phase is the premixing of the fuel and air prior
to ingestion into the combustion chamber. The second phase is the burning
of the mixture within this enclosed chamber.
                                                                      43

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Formation and Control of Combustion Pollutants

      The premixing phase can result in the subsequent formation of one or
more pollutants as a consequence of: (a) the air/fuel ratio of the mixture
entering the chamber deviates from the ratio needed for complete
combustion, (b) a localized deviation occurs in part of the mixture, or (c)
deviations occur between cylinders.  These three phenomena are discussed
further in the following paragraphs.
      The air/fuel ratio of the mixture entering the engine may deviate from
the ratio that is necessary for the maximum combustion of the fuel. In the
most extreme case, combustion may not occur because the mixture is either
too rich (excessive fuel) or too lean (excessive air) to burn, and raw fuel is
emitted from the exhaust system.  If the mixture is burnable but on the rich
side, the combustion of the fuel will be decreased and CO emissions will be
increased. If the mixture is burnable but on the lean side, NO emissions may
be increased.
      The mixture that actually enters the combustion chamber may not be
homogeneous in that it varies in regard to the size and/or the distribution of
the fuel droplets.  Such a lack of homogeneity may  result in localized rich  or
lean zones that have different combustion characteristics.
      Some of the fuel droplets may  separate out of the mixture as a result of
being deposited on and "wetting" the interior surfaces of the intake system.
In carburetted or single point injection systems, wetting can occur in the
individual runners of the  intake manifold.  In multipoint injections systems,
wetting can occur at the intake port of each cylinder. Such deposition of
liquid fuel can result in mixtures with differing air/fuel ratios being delivered
to the several cylinders in the engine. The extent of such wetting depends on
a number of variables, one of the most important being the temperature of
the intake system interior surfaces. When the amount of fuel being deposited
is increasing, the mixture entering  the combustion chamber will tend to be
lean.  When the amount of deposited fuel is decreasing, the mixture entering
the combustion chamber will tend  to be rich.  These changes in composition
will tend to lead to the formation of the emissions that are associated with
each condition.
      During the second phase, or burning of the mixture, undesirable
quenching phenomena can result in  the emission of unburned fuel.  The
44

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                                                            Appendix One

expanding ball of flame can be quenched, or extinguished, as a result of the
approach of the flame front to the relatively cool walls of the combustion
chamber or a restriction which impedes further propagation. In either case,
the quenching of the flame results in the emission of unburned fuel from the
combustion chamber.
      In compression-ignition engines, the problems of the spark-ignition
engine are avoided by the direct injection of the fuel into a volume of high
temperature air and the resultant spontaneous ignition of the fuel.
Consequently, compression-ignition engines are less subject to HC and CO
emission formation than spark-ignition engines.  However, the compression-
ignition combustion process involves phenomena which can result in the
formation of NO and/or smoke emissions.
      In both spark-ignition and compression-ignition engines, NO
formation is quite different than HC and CO formation in that NO is not a by-
product of fuel combustion. In internal combustion engines, NO formation
is a result of the  "fixation" of atmospheric nitrogen.  In open type burning
atmospheric nitrogen acts as an unreactive  diluent gas. However, the high
temperatures and pressures that are developed in the cylinders of the spark-
ignition, and to a greater degree in the cylinders of compression-ignition
engines, result in the oxidation of the atmospheric nitrogen.
      In compression-ignition engines, any incomplete oxidation of the
carbon atoms in  the fuel molecules tends to result in particulate emissions
rather than HC and/or CO emissions as is the case with spark-ignition
engines.  In compression-ignition engines, the continuous spontaneous
combustion of the fuel minimizes the possibility of fuel hydrocarbon
molecules being completely excluded from  the combustion process, as is the
case with spark-ignition engines when flame  quenching occurs.
Furthermore, such continuous spontaneous combustion in cylinders of a
compression-ignition engine which originally ingested fuel-free air, rather
than an air/fuel  mixture, eliminates  CO formation occurring when an spark-
ignition engine is operated under rich conditions (excess fuel).  A number of
factors unique to compression-ignition engines, such as the longer carbon
chains in the fuel hydrocarbons, the  higher initial temperatures and pressures
in the combustion chambers, and the spontaneous ignition of fuel that is
injected into a volume of hot air, result in compression-ignition engines
                                                                     45

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Formation and Control of Combustion Pollutants

emitting fuel carbon in the form of elemental carbon particles, rather than in
the form of unburned fuel or CO as is the case with spark-ignition engines.
Under certain conditions, such as the severe overfueling of a heavy-duty
compression-ignition engine, the emission of carbon particles becomes visibly
evident as a plume of black smoke.
46

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                  Appendix 2. Hydrocarbon Classes

      Various distillation and extraction processes can be used to separate the
hydrocarbons in raw petroleum into fractions with specific uses. All these
hydrocarbon compounds are comprised of only two kinds of atoms, carbon
and hydrogen.  Each carbon atom has four positions for attachment of
hydrogen atoms or other carbon atoms. As a consequence, the carbon atoms
can be connected together in a great many ways.
      The paraffin (alkane) hydrocarbons are saturated in that their
molecules contain the maximum possible number of hydrogen atoms.  The
paraffin hydrocarbon atoms can be arranged in three ways. Normal paraffins
have the carbon atoms connected to each other in straight chains (see figure).
Isoparaffins have isomeric structures in which side chains of carbon atoms
are attached to primary chains (see figure).  Cycloparaffins have the carbon
atoms arranged in closed chains or rings (see figure). The three types of
paraffins comprise about 50% or more of the hydrocarbons in gasoline and
about 35% of the hydrocarbons in exhaust gases.
      The alkene or olefin hydrocarbons are unsaturated in that double
bonds between two adjacent carbon atoms eliminate two sites for the
attachment of hydrogen atoms (see figure).  Like  the paraffins, the olefins can
have branched chain isomers.  The olefins can also have the carbon atoms
connected in closed rings.  The olefins are rare in "straight run" gasoline
which are produced by the simple distillation of raw petroleum. However,
olefins are present in considerable quantity in highly "cracked" gasoline
which are produced by refining processes that break or crack hydrocarbon
molecules with long carbon chains.  Olefins comprise as much as 10% of the
hydrocarbons in gasoline and about 45% of the hydrocarbons in exhaust gases.
      The aromatic hydrocarbons have one or more benzene rings in their
molecular configuration.  The unique benzene molecule is in the form of a
closed ring in which six carbon atoms are connected by alternating  single and
double bonds. Aromatic hydrocarbons are found in crude petroleum and are
the predominant hydrocarbon class in coal distillation  products. Aromatic
hydrocarbons comprise about 40% of the hydrocarbons in gasoline and 20% of
the hydrocarbons in exhaust gases.
                                                                     47

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Formation and Control of Combustion Pollutants
      The oxygenated organic compounds have one or more oxygen atoms
directly attached to the carbon atoms in their molecules (see figure).  The
various types of oxygenated organic compounds are alcohols, ethers,
aldehydes, ketones, carboxylic acids, and esters.
      If the carbon atoms are connected together to form straight open
chains, the general formula is CnH2n + 2, where n is the number of carbon
atoms in the chain. If carbon atoms in side chains are present, as in the
paraffin isomers or isoparaffins, the same general formula is applicable. If the
carbon atoms are arranged in closed chains or rings, as is the case with the
cycloparaffins, the general formula is CnH2n .  When there is only one double
bond in the molecule, the general formula is CnH2n .
Paraffin (Alkane) Hydrocarbons (Saturated Straight Chain)
      The first five hydrocarbons in the series are shown. Each terminal
carbon atom has three attached hydrocarbon atoms and each interior carbon
atom has two attached hydrocarbon atoms.  In their pure isolated state, the
first four members of the series; methane, ethane, propane, and butane, are in
a gaseous state at standard temperature and pressure conditions.
              "
H-i
     i
-H      H-
                   H  H
                  C-t-H
                  A  A
                  Ethane
                                                H   H  H
                                            H-t-C-C-H
                                                A   li  A
            Methane
                                                  Propane
H   H   H  H
H  A   H  A
    Butane
                                        H  H   H   H  H
                                        H  H       H H
                                             Pentane
Isoparaffin (Alkane) Hydrocarbons (Saturated, Branched Chain)
      Three different isomers are shown which have branched chains and at
least one carbon atom in the molecule is attached to three other carbon atoms.
Isobutane, the first member in the series, shows that a minimum of four
48

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                                                            Appendix Two
carbon atoms is necessary for chain branching. The two octane isomers show
how configurations can vary when large molecules are involved.
                                                    H      H
                      H  H  H  H  H  H  H
                   H-C-C-C-C-C-C-C-H
                            H  H  H  H  H
     H  H  H
  H-C-C-C-H
     H
H
      H-C-H
        i
        H
Isobutane (2-methyl propane)
H
              H-C-H
                 i
                 H
               Isooctane (2-methyl heptane)
    H-C-H H-C-H
  H    I  H      "
H-C—(-C-C—C-H
  _L    lit    i
                 H
                          H    1   H
                            H-C-H
                              H
                          Isooctane (2,2,4-trimethyl pentane)
  Cycloparaffin (Alkane) Hydrocarbons (Saturated, Closed Ring)
        Two closed ring cyclohydrocarbon molecules are shown. The
  cyclopropane molecule shows that a minimum of three carbon atoms are
  necessary. The methylcyclobutane molecule shows how another structure,
  such as a straight chain, can be attached to a closed ring.
                                             H
                                         H-t-H
                    H
                 H'
                  Cyclopropane
                               HO    '
-------
Formation and Control of Combustion Pollutants
          X

                I \ /•
                c=c
                    H
                Ethene

              H H  H H
            H-C-C=C-C-H
              H      H
                Butene-2
                                  H HH  H
                               H-C=C-C-C-H
                                       HH
                                   Butene-1
                                  H  H H H
                                   Butadiene
Hydrocarbons with Six Carbon Atoms

     Five of the ways are shown in which six. carbon atoms can be arranged
in isomeric molecular configurations. The-benzene molecule, with its
combination of single and double bonds, is a unique configuration. It has
distinctive characteristics, such as an aromatic odor and a tendency to burn
with a smoky flame.
    H  H  H  H  H  H
H-C-C-li-C-C-li-H
    i   i   i    i    ii
    H  H  H  H  H  H
           Hexane

    H  H  H  H  H
                                   H  H  H  H   H  H
                               H-c=ii-c-i!:-c-d-H
                                          H  H   H  H
                                         Hexene
     I   I    I   I    I
    H  |   H  H  H
     H-C-H
       H
       lsohexane-2
                                                    H
                                ^  ,
                                HAH H
                              Cyclohexane
                                                  Benzene
50

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                                                         Appendix Two

Oxygenated Organic Compounds
      Two ways are shown in which oxygen atoms can be directly attached to
the carbon atoms in a chain.
      The alcohols have a hydroxyl (-OH) functional group attached to a
terminal or intermediate carbon atom in the chain.  The two simplest
alcohols, methanol ("wood alcohol") and ethanol ("grain alcohol"), are
shown in the figure.
                             Alcohols
                       H              H  H
                    H-fc-OH      H-i-i-OH
                       A              A  A
                     Methanol          Ethanol
      The ethers have an oxygen atom which serves as the connecting link
between two carbon chains.  The two simplest ethers, dimethyl ether  and
methyl ethyl ether are shown in the figure.
                             Ethers
                                      H     H  H
                                   H-C-0-fc-C-H
                  t-o-fc-H     H-C-0-fc-C
                  A      A            A     A   A
                 Dimethyl ether           Methy| ethy| ethef

      In some molecules, an oxygen atom replaces two hydrogen atoms by
double bonding with a carbon atom to form a carbonyl (C=O) functional
group. When the carbonyl group is attached to a terminal carbon atom at the
end of a chain, the resulting compound is called an aldehyde. When the
carbonyl group is attached to  a carbon atom that is connected .to two other
carbon atoms, the resulting compound is called a ketone. The simplest forms
of aldehydes and ketones are  shown in the figure.
                                                                 51

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Formation and Control of Combustion Pollutants

         Aldehydes                                Ketones

    H                H  H             H   0  H           HOHH
    t=0         H-t-t=0       H-t-B-t-H     H-fc-C-i-t
    A                A                 A      A           A      A  A
 Formaldehyde         Acetaldehyde            Acetone           Methy ethyl ketone

      The carboxylic acids can be considered to be hybrids of alcohols and
aldehydes in that a terminal carbon atom has a carbonyl group and a double
bonded oxygen atom attached to it. The two simplest acids, formic acid and
acetic acid, are shown in the figure.
                         Carboxylic Acids
                                       H  0
                       0            H-t-C-OH
                   H-C-OH          A  k
                   Formic Acid          Acetic Acid
      An ester has two carbon chains joined by a oxygen atom and one of the
carbon atoms attached to the oxygen atom also has a double bonded oxygen
attached to it. An ester can be synthesized by combining a molecule of an
carboxylic acid and a molecule of an alcohol in a manner which results in the
liberation of a molecule of water. In this respect, an ester can be considered to
be the organic equivalent of an inorganic salt, such as sodium chloride
(NaCl) which is formed when an acid, such as hydrochloric acid (HC1) reacts
with a base, such as sodium hydroxide (NaOH).  Consequently, the methyl
formate molecule in the figure can be considered to be the end product when
a methanol molecule and formic acid molecule combine. The ethyl acetate
molecule in the figure can be considered to be the end product when an
ethanol molecule and an  acetic acid molecule combine.
                HO             H  H      0   H
             H-t-0-C-OH     H-i-C-0-C -C-H
                A                    A  A          A
              Methyl Formate                Ethyl Acetate
52

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