Environmental Protection Technology Series
INFRARED  ABSORPTION  BY
      SULFURIC ACID  VAPOR
         Environmental Sciences Research Laboratory
              Office of Research and Development
              U.S. Environmental Protection Agency
        Research Triangle Park, North Carolina 27711

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                 RESEARCH REPORTING SERIES

 Research reports of the Office of Research and Development, U.S. Environmental
 Protection Agency, have been grouped into  five series. These five broad
 categories were established to facilitate further development and application of
 environmental technology. Elimination of traditional grouping was consciously
 planned to foster technology transfer and a maximum interface in related fields.
 The five series are:

     1.    Environmental Health Effects Research
     2.    Environmental Protection Technology
     3.    Ecological Research
     4.    Environmental Monitoring
     5.    Socioeconomic Environmental  Studies

 This report has  been assigned to  the ENVIRONMENTAL PROTECTION
 TECHNOLOGY series. This series describes research performed to develop and
 demonstrate instrumentation,  equipment, and methodology to  repair or prevent
 environmental degradation from point and non-point sources  of pollution. This
 work provides the new or improved technology required for the control  and
 treatment of pollution sources to meet environmental quality standards.
This document is available to the public through the National Technical Informa-
tion Service, Springfield, Virginia 22161.

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                                            EPA-600/2-76-191
                                            July 1976
   INFRARED ABSORPTION BY SULFURIC ACID VAPOR
                       by
       Darrell E. Burch, Francis J. Gates
               and Norman Potter
          Aeronutronic Ford Corporation
              Aeronutronic Division
         Newport Beach, California 92663
                   Contract No.

                    68-02-1774



                  Project Officer

                 Roosevelt Rollins
Emission Measurement and Characterization Division
    Environmental Sciences Research Laboratory
   Research Triangle Park, North Carolina 27711
    ENVIRONMENTAL SCIENCES RESEARCH LABORATORY
        OFFICE OF RESEARCH AND DEVELOPMENT
       U.S.  ENVIRONMENTAL PROTECTION AGENCY
   RESEARCH TRIANGLE PARK, NORTH CAROLINA 27711

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                              DISCLAIMER
This report has been reviewed by the Environmental Sciences Research
Laboratory, U.S. Environmental Protection Agency, and approved for
publication.  Approval does not signify that the contents necessarily
reflect the views and policies of the U.S. Environmental Protection
Agency, nor does mention of trade names or commercial products con-
stitute endorsement or recommendation for use.
                                  ii

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                                   ABSTRACT
A sample cell has been designed and built to contain hot l^SO^ vapor for spec-
troscopic analysis.  The cell is heated to between 190° and 250°C by an electric
furnace designed specifically for use with the sample cell.  A small bulb con-
nected to the main compartment of the sample cell contains liquid l^SO^.  The
partial pressure of the t^SO^ vapor is controlled by regulating the temperature
of the liquid 112804, which is at lower temperature than any other part of the
cell that is in contact with the vapor.  Transmission curves have been scanned
for a variety of samples over the 7.8 g.m - 12.8 |j,m region with spectral slit-
widths between 0.5 cm'l and 4 cm" .  At wavelengths of maximum absorption near
8.2 M,m and 11.4 urn, the absorption coefficient is approximately 0.0004  (ppm -
meters)""^.
                                      iii

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iv

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                                     CONTENTS




                                                                         Page






Abstract                                                                  ±±±




Figures                                                                    vi






I       Introduction                                                        1




II      Summary                                                             4




III     Conclusions                                                         5




IV      Recommendations                                                     7




V       Experimental Apparatus and Methods                                 10




VI      Results of Transmission Measurements                               18

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                                    FIGURES
Number
        Optical diagram of the apparatus used to study hot H_SO
2
3
4
5
6
7
8

Two views of the sample cell. .
End view showing the location of
t. "r

the silicon windows and the
Side view of the furnace with the sample cell in place 	
Spectral curves of transmittance for three samples of H,,SO, . .
Spectra of H.SO, and H_0 between
Spectra of H,,SO, and CO,, between
7 . 85 |im and 8 . 45 urn 	 	

11
12
14
15
19
20
21
26
                                      vi

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                                   SECTION I

                                 INTRODUCTION


Under a previous contract,  Aeronutronic Ford Corporation designed, fabricated,
tested and delivered a cross-stack monitor for either HF, HCl, CO, NO or S02
that is based on the gas-filter correlation (GFC) principle.  The instrument was
delivered to EPA in June 1974, and extensive tests performed by EPA personnel
since that time have shown that it meets design specifications for HF,  CO,  NO,
and S02.  Field evaluations have not been performed for HCl, but no problems are
anticipated.  During the field tests it was determined that a few minor modifi-
cations to the instrument would simplify the operation and improve the  performance.
It was originally intended that the instrument would also measure S03 in addition
to any of the other 5 gas species, but during the design phase it was determined
that the GFC technique is not suitable for S03 because of the difficulties  in
maintaining a known constant amount of this gas in a small cell.

The original objectives of the project reported herein were to (1) make recom-
mended modifications to the existing instrument to simplify operation and to
improve its performance, and (2) retrofit the existing instrument with  a dis-
persive correlation accessory that would allow either S02 or S03 to be  measured.
The gas of primary importance was S03; however, the capability of measuring S02
was to be included because the additional cost would be small.  Furthermore, the
expected performance for S02 was better than that obtained with the instrument
when employing the GFC technique.

Objective number 1 listed in the previous paragraph has been completed.  During
the early part of the present contract, EPA scientific personnel investigated
the complex chemical reactions involving S03 that occur in the stacks of station-
ary sources.  The results of this investigation indicated that the typical  ef-
fluent probably contains more H2S04 than S03.  Much of the S03 that is  formed
probably reacts with the H20 that is present and forms H2S04.  Thus, it was de-
cided that the need for an H2S04 monitor was greater that that for an S03 monitor.
1.  Burch, D. E., and D. A. Gryvnak.  "Infrared Gas Filter Correlation Instrument
    for In-Situ Measurement of Gaseous Pollutants."  Prepared by Philco-Ford
    Corporation for EPA under Contract No. 68-02-0575.  EPA Report No. EPA-650/2-
    74-094.  Also, Burch, D. E., and D. A. Gryvnak.  "Cross-Stack Measurement of
    Pollutant Concentrations Using Gas-Cell Correlation Spectroscopy." Chapter 10
    of Analytical Methods Applied to Air Pollution Measurements, Stevens, R. K.
    and W. F. Herget, (eds.).  Ann Arbor, Ann Arbor Science Publishers Inc., 1974.

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 Therefore, the work on the dispersive correlation accessory for 862 and SOo was
 stopped, and the effort was diverted to an investigation of a cross-stack method
 of monitoring hot HoSO^ vapor.  Possible problems in maintaining the chemical
 integrity of a sample as it is drawn through a probe to a remote monitor make
 this type of instrument much less desirable than a cross-stack instrument that
 does not disturb the sample.
       2
 Alpert  has published very high resolution spectra of E2SO^ vapor in the spectral
 region from 1312 to 1549 cm"1.  The H2S04 vapor appeared as an impurity in
 Alpert 's samples of HCN, the gas species of primary interest to him.  Alpert 's
 spectral curves show approximately 700 separate absorption lines of I^SOA, and
 the positions of more than 400 of them have been measured and tabulated to the
 nearest 0.001 cm'1.  These data are the only data known to the authors that
 show individual I^SO^ absorption lines.  The intensities of the lines are quite
 irregular, and the spacings between adjacent lines vary with an average of ap-
 proximately 0.3 cm'1.  Because of the strong absorption by H20, S02 and SOo in
 the same spectral region, this H2S04 band is of little value for monitoring
 purposes.
                          o
 Chackalackal and Stafford  have published low resolution spectra of hot H2S04
 vapor in the spectral region 400 - 4000 cm"1.  The vapor was produced by heat-
 ing the azeotropic mixture (98.37o) of liquid l^SO^.  Some S03 was also present
 in the vapor over the hot liquid; the percentage of S0
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re 90 ,^  ?9?2  4-l8?f i*     y ^ centere? near 361° cm'1  (2.77 pa),  1450 cnf1
(6 90 jun)  1224 cm'l  (8.17 ym), and 882 cm-1 (11.34 p»).  The first band  listed
overlaps strong absorption by H20 and C02.  The second band  listed ,  the  one
on which data are given in Reference 2, is also overlapped by an H20  band as
well as by S02 and S03 bands.  The 8.17 \m band and the 11.34 urn band have been
emphasized in the present study because they occur where there is much  less
absorption by gases likely to be present in samples to be investigated  for
H2S04 vapor.

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                                    SECTION II

                                     SUMMARY


 A sample cell has been designed and built to contain hot H2S04 vapor for spec-
 troscopic analysis.  The cell is heated to between 190° and 250°C by an electric
 furnace designed specifically for use with the sample cell.  A small bulb con-
 nected to the main compartment of the sample cell contains  liquid l^SO^.   The
 partial pressure of the l^SO^ vapor is controlled by regulating the temperature
 of the liquid H2SO^,  which is at lower temperature than any other part  of the
 cell that is in contact with the vapor.   Typical temperatures of the liquid
 H2S04 and of the vapor being analyzed are approximately 180°C and 210°C,  res-
 pectively.

 The main body of the  cell  is made of  glass,  and the  gasket  material used to
 provide a leak-tight  seal  is resistant to chemical reaction with the E2SO^
 vapor.   Two  silicon windows  make it possible to transmit a  monitoring beam of
 infrared radiant energy through  the hot  I^SO,  vapor.   A gold-coated spherical
 mirror  forms one end  of the  cell and  reflects  the  monitoring beam so that the
 cell is double-passed with a total  optical path length of 52 cm through the
 vapor.

 A small grating spectrometer has been employed to  scan spectral curves  of
 transmittance for several  samples over the 7 am to 13  am spectral region.  In
 addition to  the H2SC>4 vapor,  some 803 vapor  and H20  are also present in the
 sample  cell.   Two strong H2S04 bands  occur in  this region;  wavelengths  of maxi-
 mum absorption are near 8.2  am and .11.4  urn.  Adjacent  individual absorption
 lines within each band are probably separated  by only  approximately 0.3 cm"1
 as  they are  in the 6.90 am band  (see  Reference 2).   These closely spaced
 individual lines  were not resolvable  by  our  spectrometer, which  has  a minimum
 practical spectral slitwidth  of  approximately  0.4  cm'1 in this  portion  of  the
 spectrum.

The absorption by  both  the 8.2 am band and the 11.4  am band  is  quite  strong.
Approximately 250  ppm-meters  of  117804 vapor produces an average absorptance of
 10              eal  of a  few nrl
    over an interval of a few cnr  near the strongest absorption in either of
these bands.

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                                    SECTION  III

                                    CONCLUSIONS
 Hot  H2S04 vapor has  four relatively strong absorption bands between 2 urn and
 12 M-m.   The  two centered near 2.77 \ua and 6.90 p,m are probably of little value
 for monitoring  the I^SO^ concentration because of the strong H20 absorption in
 the same  spectral regions.  The other two bands, centered near  8.2  um and
 11.4  p.m, are much more promising for monitoring purposes.  Some interference
 by H20  is to be expected in the 8.2  \ua region; however, this interference can
 probably  be accounted for if the H20 concentration is known or  is also monitored.
 Interference by hot C02 might be a problem for a monitor that makes use of the
 11.4  pm  band.  This problem would probably be most serious when investigating
 the exhaust from a coal-burning power plant in which the C0? concentration may
 be as high as 10-20%.  Most of the error due to interference by  C02 can be ac-
 counted for by measuring the interference of the monitor to known concentra-
 tions of C02 and determining, by other methods, the concentration of this gas
 species in the gas being monitored.

 Although the absorption by H2S04 is quite strong, the absorption spectrum does
 not contain distinct, strong, well-separated features that make infrared de-
 tection and discrimination simple for some gases.  From other experimental
 studies,^ we find that the individual absorption lines have quite irregular
 spacings and that the average spacing between adjacent strong lines is usually
 less tnan U.3 cm  .  Thus, any dispersing instrument designed to take advan-
 tage of the fine spectral structure must have quite good spectral resolution
 particularly for a portable field instrument.  The most promising infrared
 monitor for H2S04 would take advantage of the coarser, less-sharp, structure
 in the infrared spectrum.  Such a monitor might involve a dispersing element
 or a series of narrow-bandpass filters.  Because it employs the coarse structure
 in the spectrum, this type of instrument is more subject to interference by
 other gas species than is an instrument that makes use of several strong,
 sharp absorption features.

 Gas-filter correlation techniques are commonly employed to exploit spectral
 structure that is not resolved by the instrument.  These gas-filter correla-
 tion techniques could probably be employed successfully for H2S04 vapor ex-
 cept for the difficult problem of confining a fixed and known amount of H2S04
 vapor in the gas-filter cell, the key component of such an instrument.  The
high reactivity of the vapor makes it difficult to maintain a vacuum tight
 seal and to prevent the disappearance of the vapor as it reacts with the walls
 of the cell and with the windows.   Furthermore, the gas-filter  cell would
have to be heated in order to maintain an adequate pressure of  the H^SO^ vapor.

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Maintaining a constant gas-filter cell temperature in a field instrument is
also a difficult problem.  Because of these problems, a gas-filter correlation
instrument does not seem to be practical for I^SO,/, vapor

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                                   SECTION IV

                                 RECOMMENDATIONS
For the near future, the most promising type of infrared, cross-stack monitor
for H2S04 vapor would contain a grating as a dispersing element and would make
use of either the 8.2 u-m band or the 11.4 M-m band.  Quite good sensitivity can
be obtained by an instrument that compares the transmission in two or more
narrow spectral intervals.  If only two intervals are compared, one should be
in a region of strong absorption by l^SO^ vapor, and the other should be in a
nearby region where the absorption is much weaker.  It may be desirable to choose
two or more intervals of strong absorption and compare their combined trans-
mission to that of two or more intervals of weak absorption.

The simplest, and probably the most dependable, method of performing the desired
comparison involves using a small grating polychromator with multiple slits in
the focal plane of the instrument.  Each slit passes one of the selected narrow
spectral intervals.  A chopper located just back of the slits alternately allows
energy to pass through the slits corresponding to the intervals of strong absorp-
tion then through those corresponding to weak absorption.  A dispersive instru-
ment with sufficiently high spectral resolution to make use of the fine structure
due to lines separated by approximately 0.3 cm'l does not appear to be practical
for field monitoring.  Therefore, it is necessary to use the coarser structure
in the spectrum; there is probably little to be gained by making either spectral
interval narrower than about 4 cm'1.  (This corresponds approximately to 0.03 p-m
near 8.2 p,m and to 0.05 p,m near 11.4 p,m.)

The choice of the spectral intervals will depend as much on possible interfering
gases as on the spectral structure of the H2S04 vapor.  Minimizing interference
by H20 is essential if the 8.2 |im band is employed.  If the 11.4 p-m band is em-
ployed, the interference by H20 is much less, but there may be interference by
C02 if this gas occurs in high concentrations, as it does, for example, in the
exhaust from coal-burning power plants.  Other gases that may be present in the
sample and interfere with the measurements must also be considered.  Ammonia,
for example, absorbs strongly at many places within the 11.4 gun H2S04 band and
could interfere if it were present.  Data shown in Section VI on the absorption
by H20 can be useful in selecting the proper intervals to reduce interference
by this gas.

The instrument built previously by Aeronutronic Ford for EPA  (Reference 1) can
be adapted easily to monitor hot l^SO^ vapor by employing two or more narrow
spectral intervals as just discussed.  A grating assembly designed and built
specifically for this purpose would fit into the space used for grating assemblies
provided for other gases.  As in the assemblies built previously, the grating

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and all of the mirrors are fastened permanently into position.  Unlike the
previously built assemblies, a chopping mechanism alternately allows the pas-
sage of energy through the various slits in the retroref lector-grid assembly.
The energy transmitted through the slits returns to the grating and is undis-
persed.  After leaving the grating assembly, the energy passes on to the de-
tector.  The gas-filter cell and the rotating mirror chopper normally used are
not employed with this assembly.  The detector signal is processed by the same
two- frequency electronics that have been provided with the instrument.

This instrument with a grid-chopper is recommended primarily as a research in-
strument to obtain approximate values for the concentration of hot HoSO<  vapor
in the exhaust of various pollution sources and to investigate the problems
involved in making accurate and reliable measurements on a routine basis.  The
instrument can be tested and calibrated in the laboratory by using a heated
cell similar to the one described in Section V to contain the l^SO^ vapor.
The same cell, but with the liquid t^SO^ removed, can contain hot CC^ , 1^0, or
any other gas that might interfere with the measurement.

With little additional effort, the grating assembly can be made so it is capable
of using either the 8.2 p,m band or the 11.4 p.m band.  A multiple-slit grid
would be provided for each band, and the grid corresponding to the band not
being used would be blocked while the other was left open.  Not more than a
few minutes would be required to change from one band to the other.  Compari-
son of the results obtained with the two different bands would provide informa-
tion on the reliability of the instrument and on the interfering gases.  A
similar set of slits could also be included near 8 urn to measure the concentra-
tion of H20.  By previously measuring the interference by H20 in the I^SO^
channel, the data on the HoO concentration could be used to account for the
H20 interference.  A similar set of slits that pass two or more intervals be-
tween 10 and 11 urn might be used to measure the concentration of C02 so its
interference can be accounted for.  A single chopping mechanism could serve
for all of the suggested sets of slits that transmit between 8 pm and 12 p,m.
Only one set of slits would be used at a given time so that only one detector
would be required.

On the basis of the data shown in Section VI, we estimate that the minimum
detectable thickness of l^SO^ for an instrument like the one just described
is between 5 ppm-meters and 30 ppm-meters.  This value is limited by the un-
certainty in the amount of interference by other gases and by the available
methods of "zeroing" the instrument with no H^SO^ in the sampling path.
For the long term, the best possible infrared monitor for l^SO^ vapor would
probably contain a tunable laser that could make use of the fine structure
in the l^SO^ spectrum.  As these lasers are further developed and become more
convenient to use, they can probably be applied to l^SO^ measurements.  Before
the optimum wavelength interval for such a scanning laser can be determined,
it is essential that the spectrum of heated HoSO^ vapor in samples at 1 atm
total pressure be investigated with a spectral slitwidth less than 0.1 cnT^.
It would be better if the slitwidth was less than 0.05 cm"* so that most of
the structure could be observed.  Such measurements require a high-quality
spectrometer with good wavelength accuracy in addition to the very good reso-
lution.  A cell similar to the one described in Section V could be used to
contain the samples.

                                        8

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A few minor changes should be made in the design of the cell used to contain
hot H2SO^ for future studies.  The most important purpose of these changes is
to reduce as much as possible the amount of reactive material in contact with
the hot H2S04 vapor.  By so doing, the samples can be made purer and there
should be much less interfering absorption in the transmission curves.   The
continued usage of a glass cell body, gold-coated mirror, teflon gaskets and
silicon windows is recommended.

Better seals between the endplates and the cell body could be obtained  if the
teflon gaskets could be compressed more firmly.  In order to do this, the
thickness of the glass wall of the cell should be increased to at least 5 mm
to provide additional strength.  Teflon gaskets, preferably 0-rings, should be
used between the silicon windows and the glass endplate.  A mechanism should
be designed to press the windows firmly against the gasket without breaking
the windows.  After the cell has been assembled, any small remaining leaks
around the gaskets could be sealed with RTV, or some other pliable cement that
is relatively inert and can withstand temperatures up to 250°C.  Any small
amount of RTV that contacts the l^SO^ vapor will probably not decompose to
cause a leak or to produce a serious amount of impurity in the sample.

The thickness of the silicon windows should not exceed approximately 0.8 mm
so as to minimize the absorption by the silicon.  Because the thin windows may
be weak, it is recommended that the diameters be 2.5 cm or less to reduce the
force on the windows when the cell is evacuated.  The surface of each window
that contacts the I^SO^ vapor should not be coated with an anti-reflection
coating.  The coatings apparently react with the l^SO^ and form  a substance
that absorbs strongly in the 8 - 10 |0m region.  An anti-reflection coating on
the outside surface of each window will improve the transmission and greatly
reduce the fringes caused by optical interference between the two surfaces of
each window.  Wedging the windows slightly can also reduce, or even eliminate,
the fringes.

A teflon valve should replace the glass valve with silicon grease that  is used
on the present cell in contact with the vapor.  There is noticeable decomposi-
tion of the grease after a few hours use of the cell.  The liquid H2S04 reser-
voir connected as an appendage to the main part of the cell has worked  satis-
factorily and should be included on any future cell.  The capability of heating
the liquid independently of the main body of the cell is quite important and is
recommended.
                           REGION III LIBRARY
                           ENVIRONMENTAL PROTECTION AGSHCY

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                                    SECTION V

                        EXPERIMENTAL APPARATUS AND METHODS


 The optical arrangement employed to obtain the spectral data on H2SOA  vapor  is
 shown in Figure 1.  Radiant energy from a Nernst source is  chopped at  450  Hz
 and is directed through the sample section to a grating monochromator.  Mirror
 M2 forms an image of the source near  mirror M3, which is adjacent  to the en-
 trance window of the sample cell.   Spherical mirror  M4 forms one end of the
 sample cell and re-images the source  near mirror M5.  Spherical mirror M7
 forms another image of the source  on  the entrance slit of the grating  mono-
 chromator.

 The sample cell is enclosed within a  custom-made furnace that heats the sample
 cell to between approximately 190°C and 250°C.   The  furnace, which is  not  shown
 in Figure 1, surrounds the sample  cell  and is  placed inside a plywood  box.   The
 box contains insulation that surrounds  the furnace.   The radiant energy beam
 passes through two pieces of glass tubing that hold  the insulation away from
 the monitoring beam.   A portion of the  furnace not shown in Figure 1 holds the
 insulation away from the  monitoring beam in the region near mirrors M2 and M5.

 The monochromator is  a modified version of a Perkin-Elmer Model 99 Prism Mono-
 chromator.   The original  prism has been removed and  replaced by a  grating with
 75 lines per mm that  is used in the first order.   A  longpass interference  fil-
 ter placed near the entrance slit  eliminates overlapping orders of shorter wave-
 lengths  that are also passed by the grating.   The detector  has  a copper-doped
 germanium element and is  cooled by liquid helium.  The detector signal is ampli-
 fied  and demodulated  by a synchronous demodulator, the dc output of which  is
 recorded on a  strip-chart  recorder.  The spectral  slit-width varied from approxi-
 mately 0.5  to  4 cm"-'-.

 The construction of the sample  cell is  illustrated by  the two views shown in
 Figure 2.   The  cell is  designed to have a minimum of contact between the hot
 H2S04 vapor  and any material with  which it might  react.   It is  necessary to
 heat the  sample cell  in order to obtain,a sufficiently high pressure of the
 ^804 vapor  for  its spectrum to be  obtained.  Attached to the main body of
 the cell by  a piece of  glass tubing is  a  small  glass reservoir  that contains
 an azeotropic mixture  (98.3%) of liquid ^804  in  water.   The pressure of the
 vapor in the sample cell  is  controlled  by regulating  the  temperature of the
 liquid H2S04.  The  liquid ^SO^ is maintained a few  degrees  C cooler than any
 other part of the cell with which  the vapor comes in contact.   This  avoids
condensation on  the inside of the  sample  cell.  It is  particularly  important
that condensation be avoided on the cell windows  or  on the  gold-coated mirror.
The vapor in the sample cell contains H2S04, 803, and  H20.   The  relative abund-
ances of the vapors of  these three gas  species depend  upon  the  temperature

                                        10

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                     Plywood Box
   Source
   M2
                                                                                 Grating
                                                                              Monochromator
Figure 1.  Optical diagram of  the apparatus used  to study  hot H2S04  vapor.

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                 Glass Endplate
TC #2   Glass Cell Body
Silicon
Windows
                                                                                 TC #4
   TC 93
                                     TOP VIEW
                  Reservoir
               Heater for
                Reservoir
                          Removable Block
                                          END VIEW

          Figure 2.   Two  views  of the sample cell.
                                       12

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 and upon the amount of H_0 in the system.

 One end of the sample cell is formed by gold-coated mirror M4.   The  center  of
 curvature of this mirror is near a point midway between the centers  of  the  two
 silicon windows.  Thus, radiant energy coming from an image near one of the
 windows is refocused to form an image near the other window,  as  illustrated in
 Figure 1.  A flat teflon gasket forms the  seal between the mirror and the cylin-
 drical glass tubing that makes up the main body of the sample cell.   A  similar
 teflon gasket forms a seal between the other end of the cylindrical  tubing  and
 a glass plate that forms the opposite end  of the cell.  The glass endplate  and
 the mirror are held in place by two aluminum endplates as  illustrated in the
 upper portion of Figure 2.  Coiled springs on each of four pieces of threaded
 rod are compressed to hold the ends firmly against the cylindrical body of  the
 cell.  A flat ring of teflon placed between the aluminum endplate and the mirror
 serves as a spacer and places the force against the backside  of  the  mirror  ap-
 proximately opposite the gasket that forms the seal.   Use  of  this ring  makes the
 shear on the mirror much less than it would be if the aluminum endplate made
 contact with the center portion of the mirror.   A similar  arrangement is used
 between the glass endplate and the corresponding aluminum  endplate on the oppo-
 site end of the sample cell.

 We experienced problems in maintaining a reliable vacuum seal with the  teflon
 gaskets used as illustrated in Figure 2.   This  problem was solved by applying
 a ring of RTV sealing compound around the  gasket after it  had been installed.
 A continuous ring of RTV completely covered the portion of the teflon gasket
 exposed to the outside of the cell.   The RTV was bonded to the glass body of
 the cell and to the mirror on one end and  to the cell body and glass endplate
 on the opposite end.   The RTV sealed the leaks  around the  teflon gaskets with
 only a very small amount of it in contact  with  the hot H2SC>4  vapor.   After
 operating the cell for a few days,  we found no  evidence of degradation  of the
 RTV used around the teflon gaskets.   More  important,  there was spectral evi-
 dence of only a small amount  of an impurity in  the sample  cell that  might have
 resulted from a chemical interaction between the H2SC>4 vapor  and the RTV.

 We originally intended to employ teflon 0-rings to provide the vacuum seal
 between the silicon windows and the glass  endplate.   Because  of  problems en-
 countered in obtaining a sufficiently tight seal,  we  found a  solution that
 made use of the RTV in the manner illustrated in Figure 3.  Each 25  mm  diameter
 silicon window was placed over a circular  hole  in the glass endplate.   The
 window was  held firmly against the  glass plate  and the RTV seal  was  applied
 around the  outer edge of the  window as  indicated.   No RTV  was applied to the
 flat  portion of the window that would be in contact with the  hot H2SO^  vapor.
 Although  a  small amount  of RTV is  necessarily in contact with the H2S(>4 vapor,
 we  found  that  the  impurities  in the  sample that result from an interaction
 between the  vapor  and the RTV was  not serious when the windows were  installed
 carefully by  the method  illustrated.   In one  instance,  one  of the windows was
 not  sealed properly.   The RTV was  not  completely cured when the  sample  cell
was  evacuated,  and a  small amount  of  RTV was  forced by the  higher outside
 pressure  through  the  gap  between the  silicon  window and the glass into  the
 interior  of  the  sample cell.   When  the  cell was  heated,  the hot  H^SO^ reacted
with  the RTV and apparently formed an impurity  with a  spectrum that  interferes
with  the spectrum  of  the  H2S04.  When the  cell was  dismantled for cleaning,  it
was apparent that  the H2S04 had  reacted  strongly with  the  RTV that it had con-
 tacted.

                                        13

-------
                      Aluminum Endplate
                                   \
                          Glass End Plate
                                           RTV Seal
           Figure  3.  End view  showing  the  location  of  the  silicon
                     windows and  the method  of  sealing them.
   \

The  silicon windows that were  first intended for use are 2 mm thick and contain
an anti-reflection coating on  each surface to maximize  transmission near 10 p,m.
Although this coating is optimized for 10 u-m, it reduces reflection throughout
the  entire 7-12 gun region investigated.  Absorption by  the silicon was bothersome,
but  it did not seriously affect the quality of  the transmission data.  Fortunately,
the  most prominent silicon absorption  feature is at approximately 9 |im where it
does not interfere significantly with  either of the two strong H^SO^ absorption
bands investigated.  A thinner pair of windows, each 0.8 mm  thick, were available
in the laboratory and were used in order to reduce the  absorption by the silicon.
However, these thinner windows did not contain  an anti-reflection coating, and a
problem was created by the interference between the radiant energy reflected from
the  two parallel surfaces of each window.  This interference produced "fringes"
in the spectrum of the transmitted energy; the  fringes  were separated by approxi-
mately 2 cm'l and caused more  than 20% difference between  the maximum and the mini-
mum  transmittance.  After these tests were completed,  the  thin windows were removed,
and  the original 2 mm thick windows with anti-reflection coating were replaced on
the cell.  We then found that  the t^SO^ vapor reacted with the anti-reflection coat-
ing and produced a film on the windows that absorbed strongly between approximately
8 urn and 10 p,m.  The best data were obtained with the  thin windows and with the
monochromator slits wide enough to smooth-out the fringes produced by the windows.
A rectangular hole is cut in the aluminum endplate opposite the windows to allow
passage of the radiant energy.

The method employed to heat the body of the sample cell and the liquid reservoir
is illustrated in the lower panel of Figure 2 and in Figure 4.  The stationary
core that makes up the main part of the furnace surrounds  the body of the sample
cell and is made from aluminum square-stock approximately  3 mm thick and 100 mm
on each side.  Insulated electrical heating wire is wrapped around this alum-
inum as indicated in the figures.  The glass tubing that connects the
                                          14

-------
                                                                                                       Plywood Box
             Hoveable Core of
              Furnace
Heating Wire
Stationary Core
 of Furnace
                                                                                                        Aabeitot Sheet
Figure  4.  Side view  of the furnace  with  the  sample cell in  place.

-------
 main body of the sample cell to the liquid HoSOA  reservoir protrudes  through  a
 slot in the side of the stationary aluminum core.   This  allows  the temperature
 of the reservoir to be regulated almost independently of the temperature  of the
 main body of the cell.  The reservoir is enclosed within two cylindrical  pieces
 of ceramic tubing with a ceramic cap over the top as indicated  in the lower
 portion of Figure 2.  Heat is supplied to the reservoir  by electrical heating
 wire wrapped around the lower piece of ceramic.   Additional heating wire,  not
 shown in Figure 2, is wrapped around the glass tubing that connects the reser-
 voir to the main body of the cell.  The heating wire for the core of  the  furnace
 is illustrated in Figure 4, but not in Figure 2.

 A moveable core of the furnace was employed as indicated in Figure 4  to provide
 extra heat in the region near the silicon windows.   This short,  moveable  core
 is made of aluminum square-stock similar to that  of the  stationary core.   After
 the cell has been put in place inside of the stationary  core of  the furnace,  an
 optical assembly that contains mirrors M3 and M5  is fastened in  place and  the
 moveable core is installed.  Holes cut in the two sides  of the moveable core
 allow the light to pass through to mirror M3 and  out from mirror M5.   The  bottom
 side of the moveable core is also notched out so  that it can slide over the
 mount for the mirrors M3 and M5.

 Pieces of flat asbestos sheet, approximately 5 mm thick,  are fastened to  the  four
 sides of both the stationary core and the moveable  core  of the  furnace.   In
 addition to providing some insulation,  these asbestos plates hold the coils of
 heating wire firmly against the aluminum square-stock that forms the  cores of
 the furnace.  After the sample cell and the furnace have been installed and
 aligned, the plywood box that contains  the sample  cell and furnace is filled
 with loose insulation.   The two pieces  of glass tubing shown in  Figure 1 keep
 the insulation from interrupting the monitoring beam as  it enters and exits
 from the sample cell and furnace assembly.   When  the reservoir is to  be main-
 tained at a low temperature in order to reduce the  amount of ^SO^ vapor  in
 the cell,  the insulation is removed from around the reservoir.   With  the  insula-
 tion removed from around the reservoir  and the remainder  of the  sample heated
 to approximately 200°C,  the liquid H^O^ in the reservoir is typically at  ap-
 proximately 45 °C.

 The heating wires  are connected in five separate  circuits,  and each is con-
 trolled  independently in order to maintain the temperature of the different
 components  as desired.   One heater circuit includes the wire around the sta-
 tionary  core, one  includes  the wire around the moveable  core, and a third  is
 connected  to the moveable  block that supports  the mounts  for mirrors  M3 and M5.
 The  fourth  heater  circuit  is  shown in the lower panel of  Figure  2 and provides
 heat  to  the  liquid ^SO^ reservoir.   The fifth heater circuit is  not  shown in
 any  of the  figures;  it  includes a  few coils  of wire around the glass  tubing
 that  connects the reservoir  to  the  sample cell and  a few  coils around the  three
 glass valves and the  tubing  that  connects  them.  The power in each circuit is
 manually controlled by a variable  transformer.  Approximately 130 watts are
 required to maintain  the sample cell  at  210°C.

Figure 2 shows the location of  five  thermocouples attached  to the sample cell.
By carefully adjusting the power to  each  of  the individual heaters, it is  pos-
 sible to maintain the temperatures  indicated by thermocouples 2,  3  and 4 to
within 2°C.  Thermocouple No.  1 indicates  the  temperature  of the  liquid

                                        16

-------
 in the reservoir, which can be controlled almost independently of the other
 parts of the cell.

 In a typical experiment the sample cell is heated to approximately 210°C  with
 all of the insulation in place except for that around the reservoir so that its
 temperature remains near ambient.   Under this condition,  the vapor pressure of
 the H2S04 is so low that no absorption by the vapor can be observed with  the
 spectrometer.   Therefore, a spectral curve scanned with the cell in this  con-
 dition can serve as a 100% transmittance curve to be compared with the spectral
 curves obtained with vapor in the  cell.  When the heater for the reservoir  and
 the insulation have been put in place, the liquid H2S04 can be heated and
 stabilized in  approximately 30 minutes.

 After a series of spectral curves  have been obtained at different vapor pres-
 sures, the insulation from around  the reservoir and the heater for the reservoir
 are removed to allow the liquid to cool.   As the liquid cools, the vapor  in the
 cell condenses in the reservoir.   The decrease in the absorption is monitored
 by recording the output from the synchronous amplifier with the grating mono-
 chromator  adjusted to pass a wavelength  of strong absorption by the vapor.

The  total  pressures  of  a  few of the  samples were measured by using  the pressure
transducer shown in  Figure  1.  The  line to  the pressure transducer  and  the
volume bounded by  the three  glass valves was  filled with N2  to a pressure slightly
higher than  the  estimated pressure  in  the sample cell.  The valve to  the cell was
then  opened  for  a  few seconds  to allow a small amount  of N2  to flow into the cell
until  the  pressure in the cell was  the same as that in the transducer.  A high
impedance  recorder measured  the output of the pressure-transducer,  which had been
calibrated previously.  The  volume  filled with N2 before it  is  let  into the cell
is approximately 37.  of  the volume of the cell; therefore, the  N2 that flows into
the cell,  and thus adds to the pressure, is easily accounted for.   By following
the method described above,  the N2  in  the line served as a buffer and prevented
the flow of H2SC>4 vapor into the room-temperature pressure transducer where it
wouId c ondens e.
                                       17

-------
                                  SECTION VI

                     RESULTS  OF  TRANSMISSION  MEASUREMENTS


 Figures  5  and 6  show representative  spectral curves  of  transmission  obtained
 for  hot  H2S04 samples at  different pressures.   Background  curves  obtained with
 no H2SO^ in  the  sample cell  contained some coarse  structure  due to absorption
 by the silicon windows, spectral  variations  in  the transmission of the  inter-
 ference  filter,  and  spectral variations  in the  efficiency  of the  grating.  This
 structure  also appeared in the  original  curves  for the  H9SO,  vapor.  The curves
 in Figures 5 and 6 have been replotted on a  percent  transmittance scale to elim-
 inate the  structure  due to variations  in the background.   The physical  slitwidth
 of the spectrometer  was set at  1.2 mm, which produces a spectral  slitwidth that
 varies from  approximately 2 cm-1  at  12 |j,m to 4  cm-1  at  8 |im.   The relatively
 wide slits were  used to smooth  out the fringes  produced by the 0.8 mm thick
 silicon  windows.  The windows used at  the time  these data  were obtained did not
 contain  antireflective coatings;  thus, the optical interference between the two
 surfaces produced fringes that  were  spaced approximately 2 cm--'- apart.

 In order to  check for possible  spectral  structure  that  was not resolved by the
 2 cm"  - 4 cm"1  resolution, a few curves were scanned with spectral  slitwidths
 that varied  from approximately  0.5 cm"-'-  at 12 |im to  1 cm"1 at 8 p,m.  These data
 were obtained while  using thicker (2 mm), anti-reflection  coated  windows to
 avoid the  fringes produced by the thinner windows.   Somewhat  narrower slits
 would have been  employed  for these data,  but the GerCu  detector was  noisier than
 usual at the time so that the detector noise would have been  excessive  if nar-
 rower slits  had  been used.  The spectral curves scanned with  the  narrow, 0.5 -
 1 cm ~L, spectral slits appeared  essentially the same as those shown in Figures
 5 and 6, which were  obtained with wider  slits.  There was  only a  small, expected
 change in  the curves near the Q-branch at approximately 8.2  urn and at a few
 other similar places where the  slope of  the  curve  changes  abruptly.  The H2S04
 curve in Figure  7 contains the  8.2 |j,m  Q-branch  and was  scanned with  a spectral
 slitwidth  of approximately 1 cm-1.  No new structure was observed with  the
 narrow slits  that was  not also  observed  with the wider  slits.  It is probable
 that adjacent  lines  in much of  the spectrum  are separated  by  approximately
 0.3  cm"  ,  thus the structure due  to  individual  lines could not be observed with
 spectral slitwidths  as wide as  0.5 cm" .  Known positions  of  absorption lines
 of CH4 and NH3 were  used  for wavelength  calibration  of  the monochromator.

 Scans of the  spectra were continued beyond the  region represented in Figures 5
and 6 to approximately  7 \im.  The region between 7 |j,m and  7.8 p,m  has not been
 included in  the  figures because the curves were difficult  to  interpret quanti-
tatively.  The background curve (100%  transmittance) sloped  steeply  downward
from 7  Lj,m  to  7.8 u.m  because of  the decreasing efficiency of  the grating toward
shorter wavelengths.    In addition, the 7  - 7.8 p,m  spectrum shows  much structure
due  to  H20 in the optical path.  The extra effort  that  would  have been required
to obtain quantitative data in the 7 - 7.8 U.TO was  not considered  worthwhile in
the  present study because the strong H20 absorption  renders  this  region worthless
for monitoring l^SO^.
                                      18

-------
                            1200
                               WAVENUMBER (cm"1)

                                          1000
                                                                                         800
               100
VO
          w
I
55
                o
          Figure  5
                                  WAVELENGTH  (micrometers)

            Spectral curves of transmittance  for three samples of ^SO^.  Path length
            - 52 cm.  Vapor temperature - 235°C.  The spectral slitwidth varies from
            approximately 4 cm-1 at 8 u.m to 2 cm-1 at 12 um.  Approximate pressures
            of the lSO^ vapor are: A,  3 torr; B, 15 torr; and C, 28 torr.

-------
                      1200
         1100
  WAVENUMBER  (cm"1)




1000            900
                                                                                   800
        100
N>

o
         50
      w
      o
      H
      H
      to
                                              10             11


                                             WAVELENGTH (micrometers)
                                                    12
             Figure 6.
Spectrum of H2S04 vapor.  Path  length  = 52  cm.  Vapor  temperature

= 214°C.  H2S04 vapor pressure —  7 torr.  Spectral  slitwidth  varies

from approximately 4 cm~l at 8 u-m to 2 cm"* at  12 o,m.

-------
                                              WAVENUMBER  (cm" )
                               1250
                                                                     1200
100
Figure
                           WAVELENGTH  (micrometers)
7   Spectra of HoSO*  and H20 between 7.85  urn and 8.45  urn.   The spectral slitwidth  is approxi-
    mately 1 cm\   The  optical path length is 52 cm.   The  approximate pressures  of the gases
    are:  H?S04, 2  torr;  and H20,  600 torr.

-------
  The  7  -  7.8  p,m  region  contains a very  strong absorption band of 803 centered
  near 7.4 ^m  in  addition  to a  portion of the 6.90 (j,m H2SO, band discussed in
  Reference  2.  Strong absorption by S02 also occurs between 7.2 ^m and 7.5 ^m.
  Although this region is  difficult to interpret accurately, it does provide
  information  on  the maximun amount of 803  in the samples.  For example, sample
  C, which is  represented  in Figure 5, produced approximately 80% absorptance
  near 7.3 (j,m.  From unpublished S03 data obtained previously in our laboratory,
  we estimated that less than 1 torr of S03 would be required to produce this
  absorptance.  Some of this absorption is undoubtedly due to H2S04, and some may
  be due to  S02.  Therefore, we conclude that the partial pressure of S03 was much
  lower than the H2SO^ partial pressure in the samples studied.

  The  H20  in the approximately 4-meter optical path outside of the sample cell
  produced enough absorption in the background curve that the concentration of
  H20  in the sample cell  could not be determined from the spectra.   Little or no
  difference in the H20 absorption was observed between the sample spectra and
  the  corresponding background curves.

 Using data from the JANNAF Thermochemical  Tables^  on the equilibrium constants
  for the gases involved, we estimated the  partial  pressures of H20,  S03,  and H2S04
 vapors  over 98.3% H2SO^ liquid at the  experimental temperatures.   The  calculated
  total pressures  were typically 2-4  times  as high  as  those measured with the pres-
  sure transducer.  Although the large  discrepancy  between the  measured  and cal-
 culated pressures has not been completely  resolved,  we believe  that most of it
  is due  to erroneously high temperature  measurements  of the coolest  place in the
 cell, which determines  the vapor  pressure.   It  is  possible that  the thermocouple
 on the  liquid H2S04 reservoir  was not  in good  thermal  contact with  the liquid
 and was maintained hotter than the  liquid  because  of heat  from  reservoir heater.
 The top portion  of the  reservoir  may also  have  been  even cooler  than the liquid.
 The comparison between  the calculated and  measured pressures  suggest that the
 temperature indicated by  the  thermocouple  attached to  the  liquid  reservoir  may
 have  been as  much as  20°C too  high.

 We assumed  a  liquid H-jSO^ temperature that  corresponded to a  calculated  total
 vapor pressure equal  to that measured with the  pressure transducer.  The measured
 temperature of the main body of the sample  cell was then used to  calculate  the
 partial  pressures  of  each of the  three  gas  species for  this total pressure.   At
 the sample  cell  pressures used, H2SO^ accounted for approximately 50%  of the  total
 pressure.   Thus,  the H2S04 pressures listed for the samples represented  in  Figures
 5 and 6 are equal  to half of the measured  total pressure.  The calculated pressure
 of SO^ was  only  a  few percent  of  the total  pressure, a.  result that  agrees with the
 spectroscopic measurements near 7.3 p,m.

The primary objective has  been to obtain spectral data  on  the absorption  by an
amount of H2SO^ vapor that is reasonably well known.  Therefore, little  effort
has been devoted to investigating the equilibrium conditions.  Insufficient time
was available to investigate fully the discrepancy between the measured and cal-
culated pressures.  Impurities, including excess H^O, in the sample cell may  have
 JANNAF Thermochemical Tables, Dow Chemical Co. 1967, plus Addenda to date.
                                         22

-------
contributed slightly to the discrepancy by shifting the S03-H2S04 equilibrium.
The thermal data given in Reference 5 are believed to be reliable.

The build-up and decay of impurities in the sample cell was monitored by observ-
ing the infrared absorption.  The impurities appeared in two different forms.
Some of the impurities appeared as a deposit on the windows and on the gold-
coated mirror and remained when the cell was evacuated.  Other impurities were
mixed with the l^SO^ vapor and disappeared with the vapor when the cell was
evacuated.  The spectra of the impurities varied in shape from day to day, indi-
cating that the same species of gases were not present all of the time.  Certain
identifiable spectral features were present on some days but not on others.
After the sample cell had been cleaned, reassembled, and heated to approximately
210 - 220°C, there was little or no spectral evidence of impurities until  the
liquid l^SO^ reservoir was heated to produce I^SO. vapor.  Most of the impurities
that absorbed significantly were apparently formed by a reaction with the hot
H2SO^ vapor.

On several occasions just after spectra of the I^SO^ vapor had been scanned, the
liquid I^SO/ reservoir was cooled so that the vapor would condense.  Spectra
scanned after the vapor had condensed showed little, or no, absorption that
would be attributed to the vapor.  Some of the absorption attributed to gaseous
impurities remained after the cooling, but this disappeared when the cell was
evacuated.  Part of the absorption attributed to impurities also disappeared
when the reservoir was cooled, indicating that some of the impurities condensed
or that their presence was dependent on the presence of HoSO* vapor.

The absorption feature apparent in Figures 5 and 6 that occurs between approxi-
mately 9.4 |im and 10.1 |j,m is due primarily to a gaseous impurity that was  present
in even the cleanest samples.  The amount of this absorption varied relative to
the amount of t^SO^. vapor from one sample to another.  For example, curves B and
C of Figure 5 both show approximately the same amount of absorption at 9.7 |j,m
although there is much more H2S04 vapor in sample C than in sample B.  The shape
of the curve in Figure 6 is also seen to be different from the curves  in Figure 5
between 9.4 (j,m and 10.1 p,m.  Thus, the impurities producing this absorption were
apparently different on the two different days when the spectra were scanned.
The broken lines in Figures 5 and 6 indicate the estimated spectrum for l^SO^
vapor with no impurities.

The feature with the transmission minimum near 10.4 p,m is probably due to  t^SO^
and to some impurity.  The absorption in this region appeared to not be com-
pletely correlated with the H^SO^ pressure, but more so than the absorption  near
9.7 |j,m.  Little special effort was directed toward  isolating and identifying the
weak absorption by impurities.  The emphasis was  on the  investigation  of  strong
      absorption in spectral regions that might be useful for monitoring  the
      concentration.
The hot l^SO^ vapor apparently reacted with  the anti-reflective  coatings and
produced a substance that absorbs strongly between approximately 8 p,m  and  10 ^m.
This absorbing substance could not be wiped  or washed  from  the windows, and the
original anti-reflective coatings appeared to be  decomposed.  After  only a few
minutes of operation with hot l^SO^ vapor in the  cell,  the  absorption  between
                                      23

-------
 8 (im and  LO |j,ra could be  seen  to  increase.  This  changing absorption made it
 impractical to obtain  quantitative absorption  data  for the 8.2 pm band with
 the  anti-reflection-coated windows in  place.   The substance  deposited on the
 windows also absorbed  slightly in the  region of  the  11.4 n,m  band, but much less
 than in the region  of  the shorter wavelength band.   This substance accounts for
 some of the apparerit absorption  by I^SO^  illustrated by the  curve in Figure 7.
 The  contribution by this substance is  slight for wavelengths shorter than 8.1 p,m,
 but  it increases for longer wavelengths.

 Figure 7  contains a spectrum  of  hot H2S04 vapor  superimposed on a spectrum of
 H20  vapor and  illustrates the problem  of t^O interference if the 8.2 u-tn band
 of H2S04  is used.   Good  sensitivity to H2S04 could be obtained by an instrument
 that compares  the transmission in two  4 cm~l wide intervals, one centered near
 1223 cm-1 and  the other  centered near  1233 cm-1.  The lower  wavenumber inter-
 val  contains strong absorption and is  within the Q-branch.   The 1233 cm-1
 interval  contains weaker absorption, yet  it is close enough  to the other inter-
 val  that  the instrument  zero-setting would be  relatively insensitive to changes
 in source temperature, spectral  responsivity of  the  detector, etc.  Unfortunately,
 strong absorption by H20 coincides with the Q-branch of H2S04.  Therefore, an
 instrument that compares these two intervals would also be sensitive to H20 vapor
 because the H20 absorption is much stronger in one  interval  than in the other.

 For  best  results, the H2S04 absorption should  be quite different in the two
 intervals being compared, and the 1^0  absorption should be weak and approxi-
 mately the same in  both  intervals.  If the interval  centered near 1233 cm"l
 were to be used, the amount of 1^0 interference  could be reduced by selecting
 the  other interval  such  that  the H20 absorption  is nearly the same in both
 intervals.  A  4 cm-1 wide interval centered near 1253 cm-1 might satisfy this
 requirement for the interval  of  weak I^SO^. absorption.  The  accuracy with which
 H20  interference can be  accounted for  in this  manner is limited because the
 relative  amounts of absorption in the  two intervals  are usually dependent on
 the  amount of  1^0 and  on the gas temperature.  Thus, the intervals may be chosen
 so that the H^O absorption is matched  for one  condition, but it may not be
 matched for other temperatures or other amounts  of H^O vapor.  If an H2SC>4
 monitor is to  be designed for gases in which the H20 vapor concentration is
 quite high, it would probably be best  to choose  two  intervals containing weak
 H20  absorption, even if  the difference in the  absorption by  l^SO^ in the two
 intervals is somewhat  less than  in other pairs of intervals  that contain strong
 H20  absorption.

 Of course, the maximum sensitivity can be achieved by one interval where the
H9S04 absorption is the  strongest and  the other  outside of the band where the
absorption is negligible.  Such  a wide separation of the two intervals generally
 increases interference by other  gases, by dirt on windows, or by particulate
matter in the  sample.  The transmittance of particulate matter suspended in the
gas  or dirt that accumulates on  windows usually  changes slowly with changing
wavelength.   Therefore,  interference by either of these two  types of matter is
usually minimized by employing two closely-spaced  intervals.
                                       24

-------
A few preliminary data on C02 absorption were obtained in the spectral region
between 10 p,m and 12 urn.  Absorption by C02 is negligible near the 8.2 gun band.
The sample cell used for H2S04 was filled to 1 atm with pure C02 while the cell
was heated to 205°C.  At the absorption minimum near 11.3 \im, this COj sample
absorbed very slightly, but less than 0.5%.  Near 11.0 |im and 11.9 M-rn on
either side of the minimum, the absorption had increased to approximately 2%
and continued to increase toward both longer and shorter wavelengths.  These
data on C02 absorption have not been included because the absorption in the
region of primary interest by the largest sample is too small to illustrate the
potential interference.  In order to show the nature of the C0£ absorption, we
have included in Figure 8 a spectrum from a report previously published by us.
Superimposed on the C02 spectrum for comparison is a portion of the H2S04 curve  A
from Figure 5.  The C02 sample represented in Figure 8 was at room temperature and
consisted of 0.30 atm of pure C02 with an optical path length of 1185 meters.
This amount of C02 is much greater than would probably ever be encountered in
the effluent from a stationary source.  However, the absorption in this spectral
region by a given amount of C02 increases rapidly with increasing temperature.
As a result, a few atm meters of C02 in a 200°C stack might produce enough ab-
sorption to interfere with an H2S04 measurement that made use of the 11.4 |j,m
band.  By measuring the gas temperature and the C02 concentration, the inter-
ference could probably be accounted for.

Other gases that might interfere with an instrument using the 11.4 urn band, de-
pending on the type of pollution source being monitored, are ammonia and ethy-
lene.  The absorption by l^SO^ does not change rapidly with wavelength at any
place in the 11.4 p-m band.  Therefore, any two narrow intervals within the band
that are compared to measure the I^SO^ concentration must be well-separated and
be subject to the above mentioned disadvantages of instability and interference.
6.  Burch, D. E. "Semi-Annual Technical Report Investigation of the Absorption
    of Infrared Radiation by Atmospheric Gases."  Prepared by Philco-Ford
    Corporation, Report No. U-4784, for ARPA, Air Force Cambridge Research
    Laboratories under Contract No. F19628-69-C-0263, 31 January 1970.
                                       25

-------
                         WAVENUMBER (cm"1)
                        900
                                   850
800
w
    50
                     11
                                         12
                                                               13
                                WAVELENGTH
Figure 8.  Spectra of
                                   and C02 between  11 yjn and 12.5 p,m.
                                    26

-------
                                   TECHNICAL REPORT DATA
                           (Please read Instructions on the reverse before completing)
1. REPORT NO.
  EPA-600/2-76-191
                                                           3. RECIPIENT'S ACCESSION" NO.
4.TITLE ANDSUBTITLE


  INFRARED ABSORPTION BY SULFURIC ACID  VAPOR
            5. REPORT DATE
              July 1976
            6. PERFORMING ORGANIZATION CODE
7. AUTHORIS)
  Darrell  E.  Burch,  Francis J. Gates,  and  Norman Potter
                                                           8. PERFORMING ORGANIZATION REPORT NO,
               U-6200
9. PERFORMING ORGANIZATION NAME AND ADDRESS
  Aeronutronic  Division
  Aeronutronic  Ford Corporation
  Ford Road
  Newport  Beach,  California  92663
            10. PROGRAM ELEMENT NO.

               1AA010
            11. CONTRACT/GRANT
                            NO.
               68-02-1774
12. SPONSORING AGENCY NAME AND ADDRESS
                                                           13. TYPE OF REPORT AND PERIOD COVERED
  Environmental  Sciences Research  Laboratory
  Office  of  Research and Development
  U.S.  Environmental Protection Agency
  Research Triangle Park, North Carolina  27711
               Final:  R/75-1/76
             14. SPONSORING AGENCY CODE

               EPA-ORD
15. SUPPLEMENTARY NOTES
16. ABSTRACT

  A sample  cell  has been designed  and built to contain  hot  ^04 vapor for spectro-
  scopic  analysis.   The cell  is  heated to between 190°  and  250°C by an electric
  furnace designed specifically  for use with the sample cell.   A small bulb connected
  to the  main compartment of  the sample cell contains liquid H2S04-  The partial
  pressure  of the H2S04 vapor is controlled by regulating  the temperature of  the
  liquid  H2S04,  which is at lower  temperature than any  other part of the cell  that
  is in contact  with the vapor.   Transmission curves have  been scanned for a  variety
  of samples  over the 7.8 ym  - 12.8 ym region with spectral  slitwidths between 0.5
  cm"1 and  4  cnr"1.   At wavelengths of maximum absorption near 8.2 urn and 11.4
  the  absorption coefficient  is  approximately 0.0004  (ppm - meters)-!.
                                   ym.
17.
                                KEY WORDS AND DOCUMENT ANALYSIS
                  DESCRIPTORS
                                              b.lDENTIFIERS/OPEN ENDED TERMS
                             COSATI I ield/Group
  *Air  pollution
  *Sulfuric acid
  *Sulfur trioxide
  *Sulfur dioxide
  *Electromagnetic absorption
  *Infrared spectroscopy
                              13B
                              07B
                              20C
                              14B
13. DISTRIBUTION STATEMENT
  RELEASE TO PUBLIC
19. SECURITY CLASS (This Report)

  UNr.l ASSTFTFH
                                                                          21. NO. OF PAGES
20. SECURITY CLASS (This page)
  UNCLASSIFIED
                                                                          22. PRICE
EPA Form 2220-1 (9-73)
                                             27

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