United States
                   Environmental Protection
                   Agency
Air and Energy Engineering
Research Laboratory
Research Triangle Park NC 27711
                   Research and Development
EPA/600/S7-89/005 Feb.  1990
ve/EPA         Project  Summary
                   Bench-Scale  Studies  to  Identify
                   Process  Parameters  Controlling
                   Reburning  with  Pulverized  Coal

                   D. W. Pershing, M. P. Heap, and W. R. Seeker
                    The  report  addresses  the
                  evaluation of a technology which is a
                  combination of two  technologies
                  used to  control the atmospheric
                  emission of  NOX  by  stationary
                  sources: (1) combustion modification
                  (controls flame temperature  and
                  maximizes fuel-rich residence time to
                  minimize  NOX formation); and (2) flue
                  gas cleaning (uses a reducing agent
                  with or without a catalyst to remove
                  NOX from  combustion products).  The
                  combined technology uses fuel as a
                  reducing  agent to remove NOX. The
                  process (referred to  as  in-furnace
                  NOX reduction, reburning, and staged
                  fuel injection) can be applied to many
                  types of  combustion systems.  In
                  fact, reburning is the process which
                  allows the "in-furnace NOX reduction"
                  to take place.
                    This Project Summary was devel-
                  oped  by EPA's Air and Energy
                  Engineering Research  Laboratory,
                  Research Triangle Park,  NC,  to
                  announce key findings of the research
                  project  that is fully documented in a
                  separate report of the same title, (see
                  Project Report ordering Information at
                  back).

                  Introduction
                    This report summarizes the results of a
                  small theoretical and experimental study
                  which was undertaken as part of  the
                  EPA's  Fundamental Combustion
                  Research  Program to investigate  in-
                  furnace  NOX reduction  (reburning). In
                  simple terms, the reburning concept
                  involves the use of a  heat  release zone
                  (via staged fuel addition) to convert  NO
                  formed earlier in  the  main combustion
zone into some form which will ultimately
produce N2. The process takes place in
two discrete zones.
  1. NO Reduction Zone.  Here fuel is
    added to produce  CH  radicals
    which reduce part of the NO from
    the main combustion  zone to  N2,
    HCN, and NH3.
  2. X/V Oxidation Zone. Here the final
    combustion air  is added and a
    percentage of  the  total  fixed
    nitrogen (TFN) pool  (HCN +  NO
     + NH3) and char nitrogen (if any)
    are  oxidized  to NO  as the
    remaining  fuel fragments burn  to
    C02 and H20).
  Thus, NO can produce  N2 in both
zones  and the  key to reburning is  to
provide the species and temperatures
which allow this to happen. The first zone
forms  N2 but also converts NO into
species which can also be  converted to
N2 in the second zone.

Data Available
  Figure 1 shows data  obtained with coal
firing, demonstrating the overall potential
of the  reburning concept (referred to as
Mitsubishi Advanced Combustion
Technology, or MACT). This figure also
shows data  obtained in  the boiler
simulator furnace (BSF) at  Energy and
Environmental Research  Corporation.
Both sets of data indicate that it  is
possible to achieve extremely low levels
(50 ppm NOX at  6% 02) under ideal
combustion conditions; in general, it has
been possible to reproduce the Japanese
results under similar test conditions in the
U.S.   However,  the application  of
reburning  to large-scale  commercial
systems  in the  U.S., burning a wide

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range of bituminous and low-rank  coals,
is not as simple as Figure 1 suggests.  In
the reburning process NO can  produce
N2  in both zones and, to optimize the
process, it is necessary to provide the
species and temperatures which  maxi-
mize the rate of N2 formation. Some NO
is reduced to N2 in the first zone, but the
remaining NO either remains as NO or is
converted into species which are capable
of being reoxidized in the second stage.
  To  investigate  the optimization and
application of  reburning,  experimental
studies were conducted in two facilities: a
5.7 cm  ID, 7.38 MJ/hr (2kW), back-fired,
laboratory reactor firing doped  gaseous
fuels and  a  15.2 cm ID, 73.8 MJ/hr (21
kW), tunnel furnace firing pulverized coal.
The  reburning  fuels  used   in  this
investigation included  propane,  North
Dakota  lignite,  bituminous coals  from
Utah and Alabama, and Australian coal.


Conclusions
  The principal  conclusions of the  work
relate to both the NO reduction zone and
the XN oxidation zone.
NO Reduction Zone
  1.  The  optimum  rich-zone  stoichio-
     metry (SR2) is  approximately 0.9
     because  of  the tradeoff  between
     NO  reduction  and increased
     concentration of easily oxidizable N
     species.  Figure  2 compares  the
     data from  several sources and
     attests to the  consistency  of  the
     overall conclusion.  At stoichio-
     metries leaner than 0.9, the initial
     NO is  not  reduced as effectively
     perhaps because  of a lack of CH
     radicals.  At rich-zone stoichio-
     metries below approximately 0.9,
     large  amounts of  TFN  species
     (particularly HCN and NH3)  are
     produced and ultimately oxidized to
     NO in the final stage. As Figure 2
     indicates, this  problem is greatly
     enhanced with coal, where  the
     reburning fuel nitrogen becomes
     more significant as  additional
     reburning fuel is added.
  2.  The  primary zone stoichiometry
     (SR,) has little influence on  the
     exhaust  NO  at  the optimum
     reburning conditions.  Increasing
                                                       SR1 only slightly decreases
                                                       effectiveness  of  the  reburr
                                                       concept in spite of a large inc«
                                                       in the available reactive nitroge
                                                       the rich  zone  (due to increz
                                                       reburning fuel).
                                                    3.  The  nitrogen  content  of
                                                       reburning fuel  has  only  a s
                                                       effect on the reburning efficienc
                                                       optimum  combustion condith
                                                       but at lower  rich-zone stoic
                                                       metric ratios, it can  be of IT
                                                       importance.   Figure  3 shows
                                                       obtained with  doped  prop
                                                       flames and  indicates that at
                                                       zone  stoichiometries  be
                                                       approximately  0.8,  the nitre
                                                       content of the reburning fuel gn
                                                       influences the effectiveness  of
                                                       reburning concept.   This ii
                                                       particular importance becaus
                                                       large-scale  utility system  w
                                                       inevitably have a  distributioi
                                                       rich-zone stoichiometries  ac
                                                       the combustion  chamber in
                                                       reburning zone.
                                                    4.  The effectiveness  of rebur
                                                       depends  strongly  on
                           250
                           200
                           150
                        o
                        §  too
                        I
                        o
                        3   50
    Rate of Combustion:
-   Fuel:
    No. of Burner Units:
                                        BSF Data
              H50kg/h
              Taiheiyo Coal
              3 (Stages) x 4 (Corners)
                                 MACT = Mitsubishi Advanced Combustion Technology
                                 BSF = Boiler Simulator Furnace
                                       \	I	I        i	I
                                          I
                              0        1        23456

                                              O2 Concentration in Exhaust Gas, percent

                      Figure 1. NOX removal effect for coal firing.

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                         ID
                         Q.
90


00


70


60


50


40


30


20


10
                                     — — — Model Prediction (500 ppm)

                                     —— • Wendt (WOO ppm = NO/, Secondary Reduction Only)

                                     _.._ Takahashi et al. (Gas Phase, 100 ppm NO)

                                            EER Gas-Phase Data (540 ppm,
                                            EER Propane/Beulah Bench Scale (633 ppm)
                                          I _ I _ I _ I _ I
                             0.60       0.70      0.80      0.90        T.O

                                             Stoichiometry of the NO Reduction Zone
                    Figure 2. Effectiveness of reburmng-subscale data.
                                                     1.1
                                                              1.2
   relationship of  the  initial  NO
   concentration  to the  amount of
   reburning  fuel nitrogen added to
   achieve  an overall  rich-zone
   Stoichiometry of  0.9.  Figure  4
   shows that, even with optimum
   combustion conditions at low initial
   NO levels, reburning may actually
   increase exhaust  NO  emissions.
   With  an   initial  NO  level  of
   approximately  150  ppm  and  a
   typical coal  as the reburning fuel,
   the reactive nitrogen  available in
   the rich zone  increases  almost
   fivefold when the reburning fuel is
   added  to  acheive  an  overall
   Stoichiometry of 0.9.
5.  Coal  composition  is  important
   because it influences char  burnout,
   the  initial  NO  level, and  the
   freburning  fuel nitrogen content and
                speciation. Many coals commonly
                used  in  the  U.S.   for  power
                generation  may  prove  to  be
                relatively  unsuitable for reburning,
                particularly in retrofit  applications,
                because it will  not  be possible to
                effectively burn out the coal char in
                the available time.

          XN Oxidation Zone
            1.  The TXN  (total fixed nitrogen,
                including  char  N)  conversion
                depends on the XN speciation, the
                XN concentration, the  hydrocartbon
                content at the  rich-zone exhaust,
                and the thermal environment.
            2.  Low  XN  conversions  can  be
                achieved   by  tailoring   the
                temperature profile to  obtain
                selevtive reduction  of  NO  by NHj
                species in the final,  oxygen  rich
     stage.  Figure 5  summarizes the
     results obtained in the  tunnel
     furnace and  shows  the dramatic
     influence of thermal environment on
     the effectiveness  of  the reburning
     concept for two  initial  NO levels.
     This effect is believed to be directly
     related to a large decrease in the
     TFN conversion in the final stage of
     the reburning process.

  In  summary, the  overall  processes
controlling the reburning  phenomena
have been relatively well-identified  and
characterized. Although the  elementary
reactions are not fully  understood, the
key parameters have been identified and
the overall mechanisms defined. Further
work could define the influence of mixing
rates and establish the  potential impacts
of applying reburning  to  boilers  and
furnaces.

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                                                  (NO)., = 633 ppm
                   170

                   160

                   150

                   140

              1   130

              I   120

              \   1W

              S.  700

                   90

                   80

                   70

                   60

                   50

                   40.
                            0.6
0.7
0.8
SR2
0.9
1.0
Figure 3.  Effect of SR2 and reburning-fuel nitrogen content (tunnel furnace).

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                                                             * NHj.  N * 1.04%
    120
  a  80
     40
     20
                                                              SR, = 1.1

                                                              SR2 = 09
                                                              SR3 = 1.2S
                                                                         •o-
                                         I
             200    400    600   800   1000    1200
                                         (NO)p, ppm
Figure 4.  Influence of returning fuel type and primary NO level.

                                           CjHg/Seu/an
                                          2400  2600  2800  3000
          600
          500
          400
          300
          200
          too
     I           I           T
_   Open -  Normal
    Closed - Secondary Cooling
    SR, = 1.1
    SR3 = 1.25
                   0.6
               0.7
                                         0.8        0.9
                                              SR2
    Figure 5.  Effect of secondary cooling on exhaust NO emissions.
                                                 1.0
                                                            1.1

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D. W. Pershing, M. P. Heap, and W. R. Seeker are with Energy and Environmental
    Research Corp., Irvine,  CA 92714-4190.
W. Steven Lanier is the EPA Project Officer (see below).
The complete report, entitled "Bench-Scale Studies to Identify Process Parameters
  Controlling Returning with Pulverized Coal," (Order No. PB 89-200 81 Oi'AS; Cost
 $21.95, subject to change} will be available only from:
       National Technical Information Service
       5285 Port Royal Road
       Springfield, VA 22161
       Telephone: 703-487-4650
The EPA Project Officer can be contacted at:
       Air and Energy Engineering Research Laboratory
       U.S. Environmental Protection Agency
       Research Triangle Park, NC 27711
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
Official Business
Penalty for Private Use $300

EPA/600/S7-89/005
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