Reaction rate and photochemical data for atmospheric ... ·...
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Transcript of Reaction rate and photochemical data for atmospheric ... ·...
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NBS SPECIAL PUBLICATION 513
U.S. DEPARTMENT OF COMMERCE/ National Bureau of Standards
National Bureau of Standards
library, E-01 Admin. BIdg.
OCT 1 1981
1310B7
/
Reaction Rate and
Photochemical Data for
Atmospheric Chemistry - 1977
Reaction Rate and Photochemical Data for
K Atmospheric Chemistry - 1977 , ,11
'
Edited by
Robert F. Hampson, Jr. and David Garvin
National Measurement Laboratory
National Bureau of Standards
Washington, D.C. 20234
Sponsored by the
Department of Transportation
National Aeronautics & Space Administration
Office of Standard Reference Data, NBSOffice of Environmental Measurements, NBS
U.S. DEPARTMENT OF COMMERCE, Juanita M. Kreps, Secretary
Dr. Sidney Harman, Under Secretary
Jordan J. Baruch, Assistant Secretary for Science and Technology
^ NATIONAL BUREAU OF STANDARDS, Ernest Ambler, Director
Issued May 1978
Library of Congress Cataloging in Publication Data
Main entry under title:
Reaction rate and photochemical data for atmosphericchemistry, 1977.
(National Bureau of Standards special publication; 513)
Supt. of Docs, no,: CI3. 10:513
1. Atmospheric chemistry--Tables. 2. Chemical reaction,
Rate of—Tables, etc. 3. Photochemistry—Tables. I. Hampson,
Robert F. II. Garvin, David, 1923- III. United States. Dept.
of Transportation IV. United States. National Bureau of Stand-
ards. V. Series: United States. National Bureau of Standards.
Special publication ; 513.
QC100.U57 no. 513 [QC879.6] 602Ms [551.5'11] 78-606033
National Bureau of Standards Special Publication 513Nat. Bur. Stand. (U.S.) Spec. Publ. 513, 111 pages (May 1978)
CODEN: XNBSAV
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FOREWORD
The National Standard Reference Data System was established in1963 for the purpose of promoting the critical evaluation and dis-semination of numerical data of the physical sciences. The programis coordinated by the Office of Standard Reference Data of the NationalBureau of Standards, but Involves the efforts of many groups in uni-versities, government laboratories, and private industry. The primaryaim of the program is to provide compilations of critically evaluatednumerical data. These tables are published in the Journal of Physicaland Chemical Reference Data , The NSRDS-NBS Publication Series of theNational Bureau of Standards, and through other appropriate channels.
The present report consists of tables of data assembled for usein modelling the chemistry of the stratosphere. It represents contri-butions from the Chemical Kinetics Information Center, other NSRDSdata centers, and a number of individual experts. Support for thepreparation of those tables has been provided by the Department of
Transportation under the High Altitude Pollution Program, by the
National Aeronautics and Space Administration under the UpperAtmosphere Research Program, and by the Office of Standard ReferenceData, N.B.S. and the Office of Environmental Measurements, N.B.S.
David R. Lide, Jr.
Chief, Office of StandardReference Data
TABLE OF CONTENTS
Abstract 1
1. Introduction 1
„ Guide to the Table 3
3. Reaction Index 9
4. Table. Data for chemical reactions and photochemistryof neutral species 16
5. Reference List 67
Appendices ;
1. Chemical Thermodynamic Properties of SelectedMolecular Species 90
2. Conversion Tables 104
iv
Reaction Rate and Photochemical Data for Atmospheric Chemistry - 1977
R. F. Hampson, D. Garvin, Editors
A table of data for gas phase chemical reactionsand photochemistry of neutral species is presented.Specifically, it gives preferred values forreaction rate constants, photoabsorption crosssections, and quantum yields of primary photochemicalprocesses and also cites recent experimental work(to December 1977) . It is intended to provide thebasic physical chemical data needed as input datafor calculations modelling atmospheric chemistry.An auxiliary table of thermochemical data for thepertinent chemical species is given in the appendix.
Key words: Air pollution; atmospheric chemistry; chemical kinetics;data evaluation; gas phase; photoabsorption cross section; photochemistry;quantum yield; rate constant.
1. Introduction
This technical note consists of a table of data on the kineticsof chemical reactions and the photochemistry of neutral species. It
is designed for use in modelling the chemistry of the stratosphereand, to a more limited extent, the polluted troposphere and also theinterpretation of laboratory experiments. The table of rate andphotochemical data is supplemented by a table of thermochemicaldata for the species involved.
This work was supported by the High Altitude Pollution Program of theFederal Aviation Administration, U. S. Department of Transportation, bythe Upper Atmospheric Research Program of the National Aeronautics andSpace Administration, and by the Office of Standard Reference Data, N.B.S.and the Office of Environmental Measurements, N.B.S.
1
Earlier versions of this table have been issued as D. Garvin (editor)"Chemical Kinetics Data Survey IV" NBSIR 73-203 (1973); D. Garvin andR. F. Hampson (editors) "Chemical Kinetics Data Survey VII" NBSIR 74-430(1974) ; and R. F. Hampson and D. Garvin (editors) "Chemical Kinetic andPhotochemical Data for Modelling Atmospheric Chemistry" NBS TechnicalNote 866 (1975) . The table appearing in NBS Technical Note 866 was alsopublished in the U. S. Department of Transportation's Climatic ImpactAssessment Program Monograph 1 "The Natural Stratosphere of 1974"
E. Reiter, editor (1975). The present table supersedes all earlierversions .
Since the publication of NBS Technical Note 866 in 1975, a majoreffort in the evaluation of rate and photochemical data was undertakenfor the NASA chlorofluoromethane assessment by its LaboratoryMeasurements Committee of which the present editors were members. Therecommendations of this committee covering 104 chemical reactions and48 photochemical processes are given in NASA Reference Publication 1010"Chlorofluoromethanes and the Stratosphere" R. D. Hudson, editor,August 1977. These recommendations have been accepted by the editorsof this table and are given here as preferred values. Theserecommendations are indicated either by the entry [ t*NASA(1977) eval] orby the symbols [t*] immediately preceding the author's name in thereference column. The first notation is used to indicate that thecommittee has synthesized a preferred value from a consideration of
all data sets. The latter designation is used when the committee hasaccepted the results of a particular study or of an existing evaluation.
Recommended values also are given for reactions not consideredby the NASA Laboratory Measurements Committee. Some of these aredrawn from other modern rate data evaluations, and the sources areindicated in the table. Other recommendations have been preparedfor this work.
Rate data evaluation is a small but growing branch of physicalchemistry. There are more recommended rate constants than containedin this table, but it does contain most of those which are applicableto atmospheric chemistry. Evaluations and compilations of ratedata and on-going programs in these areas have been describedin the recent review paper "Evaluation and Compilation of ReactionRate Data" by R. F. Hampson and D. Garvin, Journal of PhysicalChemistry 81^, 2317-2319 (1977) . A current extensive listing of sources of
evaluated rate data, NBS List of Publications 73 "Chemical KineticsTables, Data Evaluations and Bibliographies. A Guide to the
Literature" is available on request from the NBS Chemical KineticsInformation Center.
Three sets of detailed data sheets have been published by us in the
course of preparing these tables. They are R. F. Hampson (editor)
"Survey of Photochemical and Rate Data for Twenty-eight Reactions of
Interest in Atmospheric Chemistry" J. Phys. Chem. Ref . Data 2^, 267 (1973);
2
R. F. Hampson (editor) "Chemical Kinetics Data Survey VI, NBSIR 73-207(1973); and D. Garvin (editor) "Chemical Kinetics Data Survey V"NBSIR 73-206 (1973) , all recommendations contained in them (and stillpertinent) are summarized in the present table.
We have also accepted many recommendations made by R. T. Watson in"Rate Constants for Reactions of CtO of Atmospheric Interest"
XJ. Phys. Chem. Ref . Data 6, 871 (1977) and by D. L. Baulch, et al"Evaluated Kinetic Data for High Temperature Reactions" Volume 1 (1972),Volume 2 (1973) and Volume 3 (1976), Butterworth and Co., London.
In addition to recommendations on rate and photochemical data the
table includes listings of current research results. These data listingsserve several purposes. Some simply record measurements, usually limitedin number, on reactions for which it is not yet practical to giverecommended values. Others show the data upon which a new recommendationis based. Still others show what has been done on a reaction since its
rate constant was last evaluated. These new data may support the
recommendation or suggest the need for modifications in the future.
2. Guide to the Table
2 . 1 General
This table provides current (December 1977) information on reactionrate constants, quantum yields and absorption cross sections. For manyreactions, preferred values are given. The reactions included in the
table are summarized in the index of reactions given in section 3.
Most of the important stratospheric reactions are in the tables.A number of the less important ones and some related systems areincluded, often simply for comparison.
The following remarks summarize the content of the table. It lists416 reactions and gives a preferred value of the rate constant for 194reactions; 136 based on recent reviews and 58 based on recent (1975-1977)experimental work. New data entries (1975-1977) are given for 252reactions, showing substantial activity in the study of gas kinetics.
The following principles have been used in the selection andpresentation of data:
a. Where a preferred value is given for a rate constant orphotochemical quantity, it is so indicated by an asterisk [*]
placed ahead of the entry in the reference column.
b. As indicated earlier an asterisk preceded by a dagger sjrmbol
[t"] is used to indicate those preferred values that havebeen recommended by the NASA Laboratory Measurements Committeeand published in NASA Reference Publication 1010 "Chlorof luoro-methanes and the Stratosphere" R. D. Hudson, editor, August 1977.
7>
c. Where there is a recent published evaluation of the dataand there are no newer data, the evaluation is adoptedand usually marked with an asterisk. The original datacovered by the evaluation are not listed separately.However this latter rule has not been applied when theevaluation has appeared within the past year.
d. Vfhere there is an evaluation but there are new data, bothare listed and a preferred value is indicated (marked byan asterisk)
.
e. Where desirable, the available recent data sets arelisted, and a selection is made or a preferred value is
synthesized from them.
2.2 Uncertainty in Recommended Value of a Rate Constant
The uncertainty assigned here to the recommended value of
a rate constant is given in the column "Notes and reliabilityof log k". This is an estimate by the evaluator of the absoluteaccuracy of the preferred value. It is a subjective judgmentderived from intercomparison of data sets, consideration of relatedreactions studied with the same technique, estimates of how wellthe parameters could have been controlled, and comparison withtheory. It means that in the evaluators judgment, the true valuewill lie within the indicated limits to a high level of confidence(90 to 95 percent)
.
Usually the uncertainty is indicated by the term in theexpression: logio k = C ± D. This is equivalent to the statementthat k is uncertain to a factor of F where D = logigl''' Thestatement that k has the value kg and is uncertain to a factor of
F means that ko/F < k < ko F.
Other forms used to indicate reliability are the following:
A < k < B means k lies in the range between A and B
k < (>) B means B is an upper (lower) limit
k ~ B means B is only a rough guide to value of k
k = A ± B alternative form for stating reliability limits
At times a rate constant expression is quoted from a paperwith individual uncertainties for the rate parameters as k =
(A ± a) exp(-B ± b/T) . These measures are those provided by theauthor and often are indications of precision, not overallreliability.
Some notes are in order, regarding the statement of theuncertainty in the recommended value of the rate constant forthose recommended values recommended by the NASA LaboratoryMeasurements Committee. Those recommendations were made for thelimited temperature range 200-300 K. The uncertainty is indicatedfor T = 230 K, a typical midstratospheric temperature and in somecases allowance for extrapolation from higher temperatures wasnecessary. This is why occasionally the entry consists of thevalue of a rate constant measured at 298 K, the symbols [^*]
immediately ahead of the entry in the reference column to show thatthis value has been adopted by the Committee for the temperaturerange 200-300 K, and a statement of the uncertainty in the preferredvalue at T = 230 K. This stated uncertainty will generally belarger than the uncertainty in the measured value (measured at298 K) to allow for the additional uncertainty introduced byextrapolation to T = 230 K.
For the recommendations made by the NASA Laboratory Committeethe indicated uncertainties in NASA Reference Publication 1010have been doubled in the present table in order to make thereliability statement analogous to a "95 percent confidence level".
2.3 Conventions Concerning Rate Constants
a. General Convention . Almost all of the reactions in thetable are elementary processes. For them the rate expression is
derivable from a statement of the reaction, e.g.
A + 2B ^ AB2
-d[A]/dt = -(1/2) d[B]/dt = d[AB2]/dt = k[A][B]^
Note that the stoichiometric coefficient for B, i.e. 2, appears inthe denominator before B's rate of change (which is equal to2k[A][B]2) and as a power on the right hand side.
Wherever there may be any doubt an explicit rate expressionis given.
5
b. Dissociation and Combination Reactions . Some reactionsof these types are not of integral kinetic order over thestratospheric pressure and temperature range. That is, althoughthey require an energy transfer agent, "M," they are in the"pressure fall-off region". For some such reactions we tabulaterate constants that include the effect of the energy transferagent and give rates for various altitudes. The reactions arewritten to demphasize "M," e.g.,
NO- + NOo (+M) ^ N_Oc (+M)
MHNOo ^ HO + NO
The rate expressions to be used do not have the concentration of Min them, e.g.. Rate = k[N02] [NO3] and k[HN03] respectively. Theunits given for the k's, s~l for first order, and cm+3 molecule~ls~lfor second order, are consistent with this convention.
The altitude, temperature and number density regime used inthese cases is
_3altitude/km temp./K log [M] /molecule cm
15 217 18.6020 217 18.2725 222 17.9330 227 17.5835 237 17.2640 251 16.9245 265 16.60
This table follov/s the U. S. standard atmosphere, 1976.
c. Forward and Reverse Reactions. In some cases there are nodata on a reaction of interest but there are data on the "reverse"reaction. Occasionally, for
A ^ B (f)
B -> A (r)
an evaluation will use the data on the "reverse" reaction together
with an equilibrium constant to obtain the other rate constant.
Obviously this is an approximation but it often is a useful method
of estimating non-measured physical properties.
6
i
The table contains notations to warn the reader when this
procedure has been used, such as "based on reverse reaction,"or when both reactions f_ and r^ are listed together "kf = kj-Kgq
or kj- = kj/Kgq. These expressions, which are those used
in the analyses, are based on equating the two rates at
equilibrium.
f r
kf[A] = k^[B]
K = [B]/[A] = \/\.
2.4 Convention Concerning Optical Absorption Coefficients
These are reported in the table as "absorption cross sectionsper molecule, base e". They are defined by the equations.
I/I^ = exp(-a[N]]l)
a = (l/([N]Jl))ln (I^/I)
where Iq and I are the intensities of incident and transmittedlight, a is the absorption cross section, cm2molecule~l, [N] is the
concentration of absorbers, molecules cm"^^ and I is the path length,
cm. Other definitions and units are frequently used. The terms
"absorption coefficient" and "extinction coefficient" are common.
It is always necessary to know what concentration units, path length
units and type of logarithm (base e or base 10) are used in the
definition. To convert "cross-sections" to absorption coefficientsin (atm at 273 K)-l cm"!, base e, multiply by 2.69 x 10^^.
A table of conversion factors is given in the appendix.
7
3. Arrangement of the Table
Data on a reaction appear only once in the table. The normallocation for a reaction is determined by its reactants. Each species
has been assigned a sequence number (1 to 65) as shown in the index that
follows. These sequence numbers are the same as those used in NBS TechnicalNote 866. New species have been inserted in appropriate positions andassigned sequence numbers such as 34a, 34b, etc. A reaction is filedunder the lower numbered species. That is, the reaction of ozone (7)
with an oxygen atom (1) is filed under reactions of oxygen atoms. Thenumbers for the reactants appear at the left margin of the table, pre-
ceding the statement of the reaction, e.g. 1,7 *-* ^3 ^2 ^2'"^^^^^
number pairs run in ascending order through the table.
If a reaction is not filed in the location described above, a cross
reference is given there. The most common exception is the listingtogether of data on the forward and reverse reactions of a pair,
i.e. A B, B A.
In the index that follows, bimolecular reactions are listed underboth reactants. Frequently the listing of reaction partners for a
particular species is divided into two parts by three dashes, separatingspecies earlier in the list than the species indexed from those later inthe list. Reactions of the particular species with those species listedbefore the three dashes should be sought under those reaction partners.There is no indexing of products of reactions. A few species are listedin the index for which there are no reactions in the table, in anticipationof expansion of the data set.
8
REACTION INDEX
1. 0
0(^D)
0(^S)
02(^A)
Rxn with: 0, 0("^S), 0^, 0^, N, NO, NO2, NO^, N^, N^O,
N20^, NH^, NH^, H, HO, HO2, H^, H^O, H2O2,
HNO2, ™03» S^2» ^°3* ^2^» ^^2*
OCS, CIO, BrO, OCIO, HCI, HBr, NO^Cl, CI2,
CI2O, CO, CO2, CN, CHO, CH2O, CH^, CH2NO2,
CH^ONO, CH^, C2H^, C2Hg, C^Hg, alkane,
Rxn with: O2, 0^, NO, NO2, N2, N2O, NH^, E^, E^O,
H2O2, HCI, CO2, CH^, C2Hg, CP2CI2, CPCI^
Rxn with: 0, O2, 0^, NO, NO2, N2, N2O, NH^, H2O,
CO2, CH^
Rxn with; 0, 0(^D), 0(^S)
hv, N, NO, NO2, NO^, N2, H, H2, H2O, H2O2,
HNO. SO, HS, CI, CN, CHO. CH3. CH3O
Rxn with: O2, 0^, N, NO, N2, H, SO, SO2, H2S, CO,
CF2CI2, CCI|^, CH^CI, CH2CI2, CHCl^
02(^2)
0.
Rxn with: O2, N2, H2O
Rxn with: 0, O(-^D), O(-^S), 02('^A)
hv, M, N, NO, NO2, H, HO, HO2, SO, SO2,
H2S, CI, Br, CIO, BrO, CO, CH2O, CH^,
CH^02, CH^ONO, CH^, C2H^, C^Hg, allene,
butenes, butadiene,
9
8. N Rxn with: 0, O^, 02(''"A), 0^ - - -
N, NO, NO^, HO, SO, SO^, OCIO
9. NO Rxn with: 0, 0(^D), O(-^S), 0^, 02('^A), 0^, N
hv, M, NO, NO2 + H2O, NO^, NH, NH^, H, HO
HO^, H^, H^O, H^O^, CI, CIO, BrO, OCIO,
CH^, CH^O, CH2O2
10. NO2 Rxn with: 0, 0 ( ) , O(-^S), O2, 0^, N, NO + H2O
hv, M, NO2, NO^, NH2, NH^, H, HO, HO2,
SO2, CI, CIO, CH^, CH^O, CH2O2
11. NO^ Rxn with; 0, O2, NO, NO2
hv, M, NO^, H2O, SO2
12. N2 Rxn with: 0, O(-^D), O(-^S), O2, 02(^A), 0^{-^Z) ^ - «
M, HO
13. N2O Rxn with: 0, 0(^D), 0(^S)
hv, M, H, HO, CIO, CO
14. N20^ Rxn with: 0 hv, M, H2O, SO2
15. NH Rxn with: NO - - -
16. NH Rxn with: 0, NO H, HO, H2, H2O
17. NH^ Rxn with: 0, O(-^D), 0(^S), NO2
M, H, HO, CIO10
17a.
18. H
Rxn with: H
19. HO
20
21
22
HO,
H^O
Rxn with;
Rxn with: 0, 0^, 02(^A), 0^, NO, NO^, N2O, NH^, NH^,
NpHzi
H, HO, HO^, H^O, H2O2, HNO, HNO^, HNO^,
SO2, HS, H^S, COS, OCIO, HCl, NOCl, 01^, CO,
CO2, CH^O, CH^OOH, CH^ONO, CH^Cl
0, 0^, N, NO, NO2, N^, N^O, NH^, NH^, H - - ^
M, HO, HO^, H^, D^, H^O, H2O2, HNO, HNO^,
HNO^, SO^, H^S, CI, HCl, DCl, HBr, NO^Cl,
CO, CH^O, CH^OH, CH^NO^, CH^ONO, CH^, C^H^,
C^H^, C^H^, C^Hg, C^H^Q, alkane, C^Hg,
CgH^CH^j C'F2Cl2, CFCl^j CH^Cl,
CH„C1„, CHCI3, CH.Cl.F,2 2* 3* 1 J k
0, 0^, NO, NO2, H, HO
M, HO2, H2, H2O, SO2, CI, Br, CIO, CO, CH2O,
CH2O2J C2H^, C2H^, C^Hg, C|^H-|^Q
0, 0(^D), O2, NO, NH2, HO, HO2
M, CI, CIO
0, 0(^D), 0(^S), O2, 02(^2), NO, NO^, N20^,
NH2, H, HO, HO2 SO^
Rxn with;
Rxn with;
Rxn with;
23 H2O2 Rxn with: 0, 0(^D), 0„, NO, H, HO
hv, M, CI, Br
11
24. HNO Rxn with: 0^, H, HO - - - M, HNO
25. HNO2 Rxn with: 0, H, HO - - - hv
26. HNO^ Rxn with: 0, H, HO - - - hv , M, CI
26a. S Rxn with: CS^, COS
27. SO Rxn with: 0, 0^, 0^{^^), 0^, N - - - SO, SO^
28. SO2 Rxn with: 0, O^C^A), 0^, NO^, NO^, ^2^5^
HO^ - - - CH^
29. SO^ Rxn with: 0, N, H^O, SO - - -
30. S^O Rxn with:
31. HS Rxn with: 0, 0^, H - - - HS
32. H2S Rxn with: 0, 02(''"A), 0^, H, HO - - -
33. HSO^ Rxn with:
34. H^SO^ Rxn with:
34a. CS Rxn with: 0 - - -
34b. CS^ Rxn with: 0, S - - -
34c. COS Rxn with: 0, H, S
12
35. CI Rxn with: 0^, 0^, NO, NO^, HO, HO^, H^, H^O^,
HNO^ - - - CI, OCIO, ClOO, NOCl, NO^Cl,
NO^Cl, Cl^O, CH^, C^Hg
Br Rxn with: 0^, HO^, H^O^ - - -
36. CIO
BrO
Rxn with: 0, 0^, NO, NO^, N^O, NH^, HO^,
hv, CIO, BrO, CO, CH^, C^H^, C^H^
Rxn with: 0, 0^, NO, CIO - - - BrO
37. ClOO Rxn with: CI hv, M
OCIO Rxn with: 0, N, NO, H, CI - - - hv
38. CIO. Rxn with:
39. HCl Rxn with: 0 , 0 ( D ) , H , HO - - - hv
HBr Rxn with: 0, HO - - -
40. HOCl
41. HOCIO
42. NOCl
Rxn with: hv
Rxn with
Rxn with: H, CI - - - hv
43. NO^Cl Rxn with: CI - - - hv
43a. NO^Cl Rxn with: 0, HO, CI - - - hv
44. CI, Rxn with: 0, H - - - hv
44a. Cl^O Rxn with: 0, CI - - -
13
45. CO Rxn with: 0, O^C'^A), 0^, N^O, H, HO, HO^, CIO
CH^O
46. CO^ Rxn with: 0, O(-^D), 0(^S), H - - - M
46a. CN Rxn with: 0, O2 - - -
47. CHO Rxn with: 0, 0^ - - -
48. CH^O Rxn with: 0, 0^, H, HO, HO^ - - - hv
49. CH^ Rxn with: 0, 0^, 0^, NO, NO^, SO^ - - -
50. CH^O Rxn with: 0^, NO, NO^, CO
51. CH^O^ Rxn with: 0^, NO, NO^, HO^ - - - CH^O^
52. CH^OH Rxn with: HO -
53. CH^OOH Rxn with: H - - -
54. CH^NO^ Rxn with: 0, HO - - -
CH^ONO Rxn with: 0, 0^, H, HO - - - hv
55. CH^NO^ Rxn with:
56. CH^ Rxn with: 0, 0 ( ) , 0(^S), 0^, HO, CI, CIO - -
56a. C^H^ Rxn with: HO, CIO - - -
57. C^H^ Rxn with: 0, 0^, HO, HO2, CIO - - -
14
58. C^Hg Rxn with: 0, O(-^D), HO,
*59. C^Hg Rxn with: 0, 0^, HO - -
t60. C^Hg Rxn with: 0, HO, HO^ - -
V60a. CgHg Rxn with: 0 , HO - - -
61. CP^Cl^ Rxn with: 0(^D), 02("^A),
62. CFCl^ Rxn with: 0 ( ) , HO - -
63. CC1|^ Rxn with: HO - - - hv
64. CH.Cl. Rxn with: 0, 0,,(^A), 0^,
/65. CH.Cl.P, Rxn with: HO - - -1 J k
* and higher alkenest and higher alkanesV and other aromatics/ and other halocarbons
15
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"
J. Chem. Phys. 66, 2690-2695 (1977)Whytock, D. A., Timmons, R. B. , Lee, J. H. , Michael, J. V., Payne, W. A., and
Stief, L. J., "Absolute Rate of the Reaction of e( ^P ) with HydrogenSulfide ever the Temperature Range 263 to 495 K," J. Chem. Phys. 65,2052-2 055 ( 1976 )
Wilson, Wm. E., Jr., "A Critical Review of the Gas-Phase Reaction Kineticsof the Hydroxyl Radical," J. Phys. Chem. Sef. Data 1., 535-573 ( 1972 )
Wong, E. L. , and Belles, F. E. , "Rate Measurements for the Reaction ofHydrogen Chloride and Deuterium Chloride with Atomic 6xygen," LewisResearch Center, NASA, Cleveland, Ohio, NASA Tech. Note, NASA TN-D-6495(1971); Chem. Abstr. 76:18326q (1972)
Wong, W. , and Davis, D. D., "A Flash Photolysis-Resonance Fluorescence Studyof the Reaction of Atomic Hydrogen with Molecular 6xygen: H flg * MHCg M," Int. J. Chem. Kinet. 6, 401-416 (1974)
Wu, C. H. , Morris, E. D., Jr., and Niki, H., "The Reaction of NitrogenDioxide with Bzone," J. Phys. Chem. 7Z. 2507-2511 (1973)
Wyrsch, D., Wendt, H. R., and Hunzlker , H, E,, "Modulation Kinetic Spectroscopyof Hg/Hg/eg/Ce Mixtures: Reactions of HgH and HOg," XI. Int. Symp.on Free Radicals ( Berchtesgaden-Konlgssee, Sept. 4-7, 1973 ) Paper No. 36;see also, Ber. Bunsenges. Physik. Chem. 7_8, 204 (1974)
Yaron, M. , von Engel, A., and Vidaud, P. H., "The Collislonal Quenching of02(^Ag) by Ne and COg," Chem Phys. Lett. 37, 159-161 (1976)
2^hniser, M. S. , Berquist, B. M, , and Kaufman, F,, "Kinetics of theReaction CI CH^ CH3 HCl from 200 to 500 K, " Int. J. Chem.Kinet. 10. 15-29 (1978)
88
Zahnlser. M. S. , Chang, J. S,, and Kaufman, F. , "Chlorine Nitrate:Kinetics of Formation by CIG * NQg M and of Reaction with eH,"J. Chem. Phys. 67, 997-1003 (1977)
Zahniser, M, S. , and Kaufman, Fo, "Kinetics of the Reactions of CIS with0 and with we," J. Chem. Phys. 66, 3673-3681 (1977)
Zahniser, M. S. , Kaufman, F., and Anderson, J. G., "Kinetics of the Reactionof 0H with HCl," Chem. Phys. Lett. 27, 507-510 (1974)
Zahniser, M. S. , Kaufman, F. , and Anderson, J. G., "Kinetics of the ReactionCI 63 - Cle Og," Chem. Phys. Lett 37, 226-231 (1976)
Zellner, R. , Erler, K. , and Field, D. , "Kinetics of the RecombinationReaction 6H H M Hgfl M at Low Temperatures," Symp. Combust.16th (Combustion Institute, Pittsburgh, 1977) 939-948
Zellner, R. , and Steinert, W., "Flash Photolysis Study of the Rate of theReaction 0H CH^ CH^ HgG over an Extended Temperature Range,"Int. J. Chem. Kinet. 8, 397-409 (1976)
89
APPENDIX 1.
Chemical Thermodynamic Properties of Selected Molecular Species
E. S. Domalski, D. Garvin, and D. D. Wagman
Two tables are provided showing chemical thermodynamic propertiesof selected molecular species of interest in stratospheric chemistry. In
these tables there are sufficient data for the usual calculations of
heats of reaction and equilibria.
The first table lists enthalpy and Gibbs energy of formation,entropy and heat capacity data. The information was extracted from"Selected Values of Chemical Thermodynamic Properties" (D. D. Wagman,et al, NBS Technical Note 270-3, January 1968) except as indicatedin the Notes. The thermodynamic properties tabluated are:
1. enthalpy of formation at OK and 298. 15K,
2. Gibbs energy of formation at 298. 15K,
3. enthalpy increment between OK and 298. 15K,
4. entropy at 298. 15K,
5. heat capacity at constant pressure at 298. 15K.
The values given for the heats of formation are based onexperimental thermodynamic and spectroscopic measurements except
where otherwise indicated; the values of S° , C ° and H° -H° forp zy o u
gaseous species were calculated by standard statistical-mechanicalequations, using corrections for vibrational anharmonicities
,
rotational stretching, and rotation-vibration interactions wherethese data were available.
The second table presents bond dissociation energies or bondstrengths. These usually are the enthalpies of simple bond scissionreactions. However, there are some cases in which there is a
substantial contribution from rearrangement of electronic structurein the products (reducing the bond energy)
.
The values given here for some molecules may differ slightly fromvalues adopted by the CODATA Task Group on Key Values for Thermodynamics(see CODATA Bulletin 17, published by the International Council of
Scientific Unions Committee on Data for Science and Technology,January 1976) . These differences will have no significant effect on theenthalpies or free energies of reaction calculated from the tables.
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i
Notes
1. Hampson, R. F. et al, J. Phys. Chem. Ref . Data _2, 267-312 (1973)
[Data sheet on 0^ + hv (u.v.)] p. 303.
2. Contributions of the higher electronic states of molecular oxygen
to the enthalpy, entropy, and heat capacity at 298 K are
insignificant
.
3. Stull, D. R. and Prophet, H. "JANAF Thermochemical Tables" 2nd.
ed. NSRDS-NBS 37 (1971).
4. Tsang, W. Estimated from kinetic data on the decomposition of
N2H^. Chapter 12, NBS Report 10904, 1 July 1972,
5. NBS Report 10904, 1 July 1972, pp. 239-307.
6. R. A. Fletcher and G. Pilcher, Trans Faraday Soc. 66, 794-799
(1970) provide more recent data for AHf° , 298.15 K.
7. Data obtained from Benson and O'Neal ("Kinetic Data on Gas
Phase Unimolecular Reactions", NSRDS-NBS-21, Feb 1970, page 55).
8. Heat formation value from S. W. Benson "Thermochemical
Kinetics" Second Edition, John Wiley and Sons (1976)
.
9. Values for AHf° , S° , and Cp° at 298.15 K were calculated using
the group additivity method described by Benson and O'Neal
("Kinetic Data on Gas Phase Unimolecular Reactions", NSRDS-NBS-
21, Feb. 1970, pp. 40-42).
The value for mf" [CH^ONOCg)] = -16.5 kcal mol"''" was derived
from the combustion data of Geiseler and Thierfelder (Z. physik.
Chem., N. F., 29, 248-257 (1961)), and the equilibrium data of
Leermakers and Ramsperger (J. Am. Chem. Soc. 54, 1837-1845
(1932)) for: CH30H(g) + NOC^(g) = CH30N0(g) +HC^(g).
o -1The value for ^f (CH30N02(g)) = -29.8 kcal mol was derived
from the work of Ray and Ogg (J. Phys. Chem. 63j 1522-1523
(1959)) on the enthalpy of reaction of N20^ with CH^ONO.
o -1 -1We have chosen S [CH30N02(g)] = 76.1 cal mol K based upon
low temperature thermal data of Gray and Smith (J. Chem. Soc.
1953
,
2380-2385). Calculations from microwave studies by
Dixon and Wilson (J. Chem. Phys. 35^ 191-198 (1961)) give S* =
72.15 cal mol "''"k"'''.
Davies, J. V., and Pritchard, H. 0., J. Chem. Thermodynamics
4, 23-29 (1972) provide more recent AHf° data.
Data on mf, S , Cp obtained from S. W. Benson and H. E.
O'Neal ("Kinetic Data on Gas Phase Unimolecular Reactions",
NSRDS-NBS-21, Feb. 1970, page 567).
Rossini, F. D., Pitzer, K. S., Amett, R. L., Braun, R. M.
and Pimentel, G. C, "Selected Values of Physical and Thermo-
dynamic Properties of Hydrocarbons and Related Compounds",
API Research Project 44, Carnegie Press, Pittsburgh, 1953.
98
16. AHf° data from Pittam and Pilcher (J. Chem. Soc, Faraday
Trans. I, 68, 2224-2229 (1972).
17. AHf° data frcjm R. L. Nuttall, A. H. Laufer and M. V. Kilday.,
J. Chem. Thermodynamics 3, 167-174 (1971).
18. Devore, J. A., and O'Neal, H. E., J. Phys. Chem. 73, 2644-
2648 (1969).
O19. Data on S° and C^ were obtained from Note (14), page 589;
data on AHf° came from Note (18).
20. Spectroscopic studies of N. Basco and R. D. Morse, J. Molec.
Spectres. 45, 35 (1973); R. A. Durie and D. A. Ramsay, Can.
J. Phys. 36, 35 (1958); P. A. G. O'Hare and A. C. Wahl, J.
Chem. Phys. 54, 3770 (1971); L. Andrews and J. I. Raymond,
J. Chem. Phys. 55, 3087 (1971); D. R. Johnson and F. X. Powell,
Bull. Am. Phys. Soc. 13^, 594 (1968); A. Carrington, P. N. Dyer,
and D. H. Levy, J. Chem. Phys. 47 , 1756 (1967) were examined
and used to calculate the thermodynamic properties.
21. Arkell, A., and Schwager, I., J. Am. Chem. Soc. 89, 5999
(1967); Johnston, H., Morris, E. D., and Van den Bogaerde, J.,
J. Am. Chem. Soc. _91, 7712 (1969), Clyne, M. A. A. and White,
I. F., Trans. Faraday Soc. 67., 2068 (1971).
22. Studies by D. J. Gardiner, J. Mol. Spectroscopy 38, 476 (1971)
and G. E. Herberich, R. H. Jackson, and D. J. Miller, J. Chem.
Soc. (A) 1966 , 336 were examined and the data used to calculate
the thermodynamic properties.
23. The spectroscopic data of K. 0. Christe^ C. J. Schack and
E. C. Curtis^ Inorg. Chem. 10, 1589 (1971) were used.
24. Thermal Constants of Substances (Termichesky Konstanty
Veshchestv), Vol. IV, V. P. Glushko, Editor, Moscow (1970).
25. The combustion data of A. T. Hu and G. C. Sinke, J. Chem.
Thermodynamics 1, 507-513 (1969) were used to derive AHf°
298.15 K values for CCl, , CHCl^, and CHoCl^ in the liquid state.4 3^ 2 2
26. The vaporization data of D. L. Hildenbrand and R. A. McDonald,
J. Phys. Chem. 63, 1521-1522 (1959) were used.
27. The combustion data of R. A. Fletcher and G. Pilcher, Trans.
Faraday Soc. 67, 3191-3201 (1971) were used to calculate
AHf° [CH^CKg)].
28. J. Chao, A. S. Rodgers, R. C. Wilhoit, and B. J. Zwolinski,
J. Phys. & Chem. Ref. Data 3^ 141-162 (1974) provide a recent
evaluation of the thermodynamic properties of CH^CCl^
.
29. Based on data in H. Okabe and M. Lenzi, J. Chem. Phys. 47,
5241 (1967) and in J. Masanet, A. Gilles and C. Vermeil,
J. Photochemistry 2, ^17 (1974/75).
30. Parker, V. B., Wagman, D. D., and Garvin, D. , NBSIR 75-968.
Selected thermochemical data compatible with the CODATA
recommendations, January 1976.
31. Value for heat of formation derived from equilibrium studies
reported by H. Imagawa, Denki Kagaku j^, 271 (1951).
100
32. JANAF Thermochemical Tables Supplement No. 48, June 1977.
33. Heat of formation value based on data in H. D. Knauth, H. Martin
and W. Stockmann, Z. Naturforsch. 29A, 200 (1974).
34. Wagman, D.D. Private communication.
101
Bond Dissociation Energies, at 0 K
Calculated from heats of formation in the accompanying table
Reaction kJ/mol kcal/mol Note
02 ^ 20
03-> O2 + 0
H2 -> 2H
HO ^ H + 0
HO^ ^ HO + 0
-> H + 0^
H^O ^ HO + H
H^O^ ^ 2H0
493. 59±0.4
101.4±2.
1
432.00±0.04
423.8±2.
1
280±8
210±8
493.7±0.8
207.1±2.1
117.97±0.1
24.24±0.5
103.25±0.01
101.3±0.5
67±2
50±2
118.0±0.2
49.5±0.5
^2^2 ^ +
^ N + N
NO ^ N + 0
NO^ NO + 0
NO^ ^ NO^ + 0
N2O ^- N + NO
^ N^ + 0
N^O^ NO + NO^
N„0, ^ N0„ + N0_z 4 / z
NO^ + NO^
HNO ^ H + NO
^- NH + 0
trans-HNO^ ^ HO + NO
HNO3 HO + NO2
NH ^ H + N
350±8
941.69±0.04
627.9
300.5
205±21
474. 9±4
161.3
35. 1±0.8
53.2
89.5
203
487
202
200
343
84±2
225.07±0.01
150.1
71.83
49±5
113. 5±1
38.58
8.4±0.2
12.7
21.4
48.6
116.5
48.4
47.8
82
102
Bond Dissociation Energies, D° at 0 K
Calculated from heats of formation in the accompanying table
Reaction kJ/mol kcal/mol Note
NH^ -> H + HN 366 87.4
NH^ -> NH^ + H 448 107
CO C + 0 1071.94±0.4 256.2±0.1
CO^ -> CO + 0 525.9±0.4 125.7±0.1
CHO CO + H 70 16.7
CH^O ^ CHO + H 364 87
CH^O -> CH^ + 0 378 90.4
^ H + H2CO 93 22
CH^O^ ^ CH^O +0 237 56.8
^ CH^ + 0^ 118 28.1
CH, ^ CH^ + H 432 103.24 3
CH^OOH CH^O + HO 184. 44.0
^ CH^ + HO2 276±8 66±2
CH^ONO ^ CH^ + NO2 248 59.2
CH2NO2 ^ CH^ + NO2 254 60.6
CH^ONO^ ^ CH^O + NO^ 174 41.6
^ CH^ + NO^ 341 81.6
SO S + 0 515. 4±8 123. 2±2
SO2 ^ SO + 0 547. 3±8 130.8±2.0
SO^ ^ SO2 + 0 342. 7±4 81.9±1
Note 1. Calculated for T = 298K
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106
NBS-114A (REV. 7-73)
U.S. DEPT. OF COMM.BIBLIOGRAPHIC DATA
SHEET
1. PUBLICATION OR REPORT NO.
NBS SP-513
2, Gov't AccessionNo.
3. Recipient's Accession No.
4, lIlLc. AINU oUDlllLr.
Reaction Rate and Photochemical Data forAtmospheric Chemistry - 1977
5. Publication Date
May 19786« Performing Organization Code
7. AUTHOR(S)
Robert F. Hampson, Jr., and David Garvin, Editors8. Performing Organ. Report No.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
NATIONAL BUREAU OF STANDARDSDEPARTMENT OF COMMERCE
10. Project/Task/Work Unit No.
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Department of Transportation, FAA, Washington, DC 20591N.A.S.A., Washington, DC 20546
Office of Standard Reference Data, NBS, Washington, DC 20234
Office of Environmental Measurements. NBS. Washington DC 2023^
13. Type of Report & PeriodCovered
14. Sponsoring Agency Code
15. SUPPLEMENTARY NOTES
Library of Congress Catalog Card Number; 78-6O603316. ABSTRACT (A 200-word or less tactual summary of most significant information. If document includes a significant
bibliography or literature survey, mention it here.)
A table of data for gas phase chemical reactions and photochemistry of neutralspecies is presented. Specifically, it gives preferred values for reaction rateconstants, photoabsorption cross sections, and quantum yields of primaryphotochemical processes and also cites recent experimental work (to December 1977).It is intended to provide the basic physical chemical data needed as input datafor calculations modelling atmospheric chemistry. An auxiliary table ofthermochemical data for the pertinent chemical species is given in the appendix.
17. KEY WORDS (six to twelve entries; alphabetical order; capitalize only the first letter of the first key word unless a proper
name; separated by semicolons) pollution; atmospheric chemistry; chemical kinetics;data evaluation; gas phase; photoabsorption cross section; photochemistry;quantum yield; rate constant
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