Temperature dependencies of the reactions of CO3- (H2O)0,1 and O3- with NO and NO2

Article abstract of DOI:10.1063/1.469668

We have measured temperature dependencies of the rate constants for CO3^- and O3^- reacting with NO and NO2.In addition, the temperature dependence of the CO3^- (H2O) reaction with NO was determined, and a 196 K rate constant was measured for the reaction of CO3^- (H2O) with NO2.The reactions with NO all proceed by O^- transfer to produce NO2^- .The temperature dependencies of the rate constants for the reactions of CO3^- and O3^- with NO are represented as 1.5*10^-7*T^-1.64 and 4.4*10^-7*T^-2.15 cm³ s^-1, respectively, and agree very well with previous measurements.The rate constant for the reaction of CO3^- (H2O) with NO is 4.1*10^-5*T^-2.72 cm³ s^-1.Previous measurements of the rate constants for CO3^-, CO3^- (H2O), and O3^- reacting with NO2 appear to be in error; our measured rate constants for the first two reactions are represented as 2.6*10^-5*T^-2.38 and 9.1*10^-9*T^-0.79 cm³ s^-1, respectively.The rate constant for the reaction CO3^- (H2O) with NO2 is 7.9*10^-11 cm³ s^-1 at 196 K.The reactions of CO3^- and CO3^-(H2O) with NO2 proceed by O^- transfer, producing NO3^- .While the reaction of O3^- with NO2 proceeds mainly by charge transfer at room temperature, about half the reactivity at 200 K is due to charge transfer with the remainder arising from O^- transfer.Atmospheric implications of the present results are discussed.

Full text of DOI:10.1063/1.469668

Temperature dependencies of the reactions of CO− 3(H2O)0,1 and O− 3 with NO and
NO2
Susan T. Arnold, Robert A. Morris, and A. A. Viggiano
Citation: The Journal of Chemical Physics 103, 2454 (1995); doi: 10.1063/1.469668
View online: http://dx.doi.org/10.1063/1.469668
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Temperature dependencies of the reactions of CO؊3 (H2O)0,1 and O3؊
with NO and NO2
Susan T. Arnold, Robert A. Morris, and A. A. Viggianoa)
Phillips Laboratory, Geophysics Directorate, Ionospheric Effects Division, (GPID), Hanscom AFB,
Massachusetts 01731-3010
͑Received 31 January 1995; accepted 9 May 1995͒
We have measured temperature dependencies of the rate constants for COϪ3 and O3Ϫ reacting with
NO and NO2. In addition, the temperature dependence of the COϪ3 ͑H2O͒ reaction with NO was
determined, and a 196 K rate constant was measured for the reaction of COϪ3 ͑H2O͒ with NO2. The
reactions with NO all proceed by OϪ transfer to produce NOϪ2 . The temperature dependencies of the
rate constants for the reactions of COϪ3 and O3Ϫ with NO are represented as 1.5ϫ10Ϫ7
and
Ϫ1.64
*
T
4.4ϫ10Ϫ7
T
cm3 sϪ1, respectively, and agree very well with previous measurements. The rate
Ϫ2.15
*
constant for the reaction of COϪ3 ͑H2O͒ with NO is 4.1ϫ10Ϫ5
cm3 sϪ1. Previous
Ϫ2.72
*
T
measurements of the rate constants for COϪ3 , CO3Ϫ͑H2O͒, and O3Ϫ reacting with NO2 appear to be in
Ϫ2.38
error; our measured rate constants for the first two reactions are represented as 2.6ϫ10Ϫ5
T
*
and 9.1ϫ10Ϫ9
cm3 sϪ1, respectively. The rate constant for the reaction COϪ3 ͑H2O͒ with NO2
Ϫ0.79
*
T
is 7.9ϫ10Ϫ11 cm3 sϪ1 at 196 K. The reactions of CO3Ϫ and COϪ3 ͑H2O͒ with NO2 proceed by OϪ
transfer, producing NOϪ3 . While the reaction of O3Ϫ with NO2 proceeds mainly by charge transfer at
room temperature, about half the reactivity at 200 K is due to charge transfer with the remainder
arising from OϪ transfer. Atmospheric implications of the present results are discussed. © 1995
American Institute of Physics.
INTRODUCTION
selected ion flow tube, which allows for a more accurate
determination of product ions than in the flowing afterglow
measurement. In this study, we have also examined the tem-
perature dependence for the reactions of OϪ3 with NO and
NO2, reactions which play a minor role in atmospheric ion
chemistry.6
Recently, Arnold and co-workers have reported a chemi-
cal ionization technique for deriving NO and NO2 concen-
trations in the atmosphere, particularly in the plumes of air-
craft where the concentrations of these compounds are
relatively large.1,2 The technique involves producing
COϪ3 ͑H2O͒ reactant ions in a flow tube which samples the
0,1
atmosphere and monitoring the product ions NOϪ2 , NO3Ϫ,
and their hydrates. The important reactions are
EXPERIMENT
The measurements were made in a variable temperature
selected ion flow tube. The apparatus has been described in
detail previously,7,8 and only details pertinent to the present
experiments are presented here. The ions COϪ3 and O3Ϫ were
formed in an electron impact ion source from CO2 and O2
source gases, respectively, while COϪ3 ͑H2O͒ was produced
from a mixture of CO2 and H2O vapor.
The NO reactant gas was added into the system through
a molecular sieve trap which was cooled to 205 K to remove
minor NO2 and HNO3 impurities. The NO2 reactant was
added directly into the flow tube. However, to prevent the
NO2 from freezing in the reactant gas inlet, it was necessary
to heat the inlet lines when cooling the flow tube. This tech-
nique has been described previously.9 Even when heating the
inlet lines, freezing prevented our working with NO2 at tem-
peratures significantly below 200 K.
There were particular experimental difficulties associ-
ated with studying reactions of COϪ3 ͑H2O͒. For example,
HCOϪ3 ͑H2O͒ and HCOϪ4 ions were produced more easily in
the ion source than was COϪ3 ͑H2O͒ under the same condi-
tions. Thus, high mass resolution was required on the up-
stream quadrupole, which significantly reduced the ion sig-
nal. The identity of the ion could be ascertained because
breakup on injection yielded COϪ3 . Only very mild injection
COϪ3 ͑H2O͒0,1ϩNO→NO2ϪϩCO2ϩ͑0,1͒H2O,
COϪ3 ͑H2O͒0,1ϩNO2→NO3ϪϩCO2ϩ͑0,1͒H2O,
͑1͒
͑2͒
where hydration of the product ion is also possible. Deriva-
tion of NO and NO2 concentrations requires a knowledge of
the rate constants for the above reactions at the temperatures
of interest, namely those at airplane cruise heights, i.e., 200–
220 K.
Rate constants for these reactions have previously been
measured at room temperature only,3,4 except for the reaction
of COϪ3 with NO for which temperature and kinetic energy
dependencies were measured at the NOAA laboratory in a
flowing afterglow.5 Since these reactions are inefficient and
such reactions generally have temperature dependent rate
constants, we have performed a temperature dependence
study of these reactions. In general, we have studied the re-
actions from 100 to 500 K. However, for experimental rea-
sons, the reaction of NO2 with COϪ3 ͑H2O͒ could only be
studied at 200 K, a temperature close to that at airplane
cruise altitudes. The present measurements were made in a
a͒
Author to whom correspondence should be addressed.
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Arnold, Morris, and Viggiano: Reactions with NO and NO2
2455
FIG. 2. Rate constants for the reactions of COϪ3 and O3Ϫ reacting with NO2
as a function of temperature. The present data are shown as solid circles and
squares, respectively. Previous data from the NOAA laboratory ͑Refs. 3 and
4͒ are shown as open circles and squares, respectively. Power law depen-
dencies for the present data are shown as dashed lines.
FIG. 1. Rate constants for the reactions of COϪ3 and O3Ϫ reacting with NO as
a function of temperature. The present data are shown as solid circles and
squares, respectively. Previous data from the NOAA laboratory ͑Refs. 3 and
5͒ are shown as open circles and squares, respectively. Power law depen-
dencies for the present data are shown as dashed lines. The power law
dependence for the OϪ3 reaction does not include the highest temperature
data point ͑see text͒.
Ϫ1.64
kCO ϩNOϭ1.5ϫ10Ϫ7
T
,
͑3͒
͑4͒
Ϫ
3
*
conditions resulted in a large percent of the ion signal re-
maining as COϪ3 ͑H2O͒.
Ϫ2.15
kO ϩNOϭ4.4ϫ10Ϫ7
T
.
Ϫ
*
3
In addition, COϪ3 ͑H2O͒ could not be studied at tempera-
tures much above 200 K, due to thermal dissociation of the
COϪ3 ͑H2O͒ ions at higher temperatures.9 Measurements in-
volving COϪ3 ͑H2O͒ ions also required the use of a hydrogen
buffer gas, which yields a lower center-of-mass collision en-
ergy for the same laboratory ion injection energy. This results
in less dissociation from the initial collisions of the ions with
the buffer.10 Despite these difficulties, it was still possible to
obtain several hundred counts per second of this ion
at 200 K.
All power law expressions in this paper contain an extra digit
in the exponent to prevent roundoff error, i.e., only the first
digit following the decimal point is significant. The OϪ3 ex-
pression excluded the highest temperature data point. The
low temperatures data ͑р300 K͒, which correspond to the
important temperature range for the atmosphere, follow the
power law very well. Thus, it is inconsequential for atmo-
spheric applications whether or not the highest temperature
data point is affected by impurities.
Rate constants for the reactions of COϪ3 and O3Ϫ reacting
with NO2 are shown in Fig. 2 as a function of temperature.
Power law dependencies are shown as dashed lines. As was
the case for NO, the reactions with NO2 are also inefficient.
However, in contrast to the NO reactions, in which CO3Ϫ
reacts faster than O3Ϫ, the reaction of O3Ϫ with NO2 is several
times faster than the reaction of COϪ3 with NO2. A likely
explanation for this is that the COϪ3 reaction proceeds exclu-
sively by OϪ transfer to produce NO3Ϫ, whereas the OϪ3 re-
action proceeds both by OϪ transfer and by charge transfer,
forming NOϪ3 and NOϪ2 , respectively,
RESULTS AND DISCUSSION
Rate constants for the reactions of COϪ3 and O3Ϫ reacting
with NO are shown in Fig. 1 as a function of temperature.
Both reactions are inefficient and proceed exclusively by OϪ
transfer to produce NO2Ϫ. The rate constant for COϪ3 is ap-
proximately 5 times larger than that for OϪ3 . Power law de-
pendencies, excluding the highest temperature point for the
OϪ3 reaction, are shown as dashed lines in the figure. The
highest temperature point for the OϪ3 reaction is plotted as an
upper limit since we could not be sure whether a small im-
purity in the NO reactant gas was affecting the measured rate
constant. This point lies slightly above the power law depen-
dence given by the other data points. Also plotted in Fig. 1
are the previous results from NOAA.5 There is excellent
agreement between the present measurements and those from
NOAA, the data being essentially indistinguishable, except
possibly for the 500 K point for COϪ3 .
OϪ3 ϩNO2→NO2ϪϩO3 ⌬HϭϪ16 kJ molϪ1
→NOϪ3 ϩO2 ⌬HϭϪ280 kJ molϪ1
.
͑5͒
The thermochemistry is from Lias et al.11 except for the elec-
tron affinity of NO2, which was taken from Ervin et al.12
The percentage of NOϪ3 produced in reaction ͑5͒ is
shown in Fig. 3 as a function of temperature. While the re-
action proceeds almost entirely by charge transfer at 500 K,
roughly half of the product ions at 200 K are NOϪ3 demon-
strating a rather strong dependence of the branching ratio on
temperature. A power dependence is shown as the dashed
line in Fig. 3 and is represented as
The temperature dependencies of these two reactions are
similar. For atmospheric purposes ͑temperatures of 300 K
and below͒, we recommend the following power law expres-
sions for the rate constants:
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2456
Arnold, Morris, and Viggiano: Reactions with NO and NO2
relatively good agreement with the data shown in Fig. 3,
especially considering that the two techniques have differing
energy distributions. The lowest kinetic energy in their ex-
periments corresponds to a temperature of about 400 K.
In general, thermal rate constants measured in a SIFT are
more reliable than those measured in either a flowing after-
glow or a beam apparatus. Beam data suffer from collection
efficiency problems and nonthermal energy distributions, es-
pecially at low energy. The flowing afterglow, although simi-
lar to a SIFT, has the disadvantage of having multiple gases
and multiple ions present in the flow tube at the same time.
To account for the differences between our measure-
ments and those made previously, we have considered the
possibility that there were dimers or other impurities in the
NO2 reactant gas. To discount the possibility of interference
by NO2 dimers, we made measurements using a dilute gas
mixture, in which the partial pressure of NO2 in the sample
reservoir was kept low ͑10–30 Torr͒. We found no measur-
able difference between neat NO2 and the dilute mixture. We
do not feel that other impurities should be a problem in our
results either. We synthesized a sample of NO2 ͑from NO
and O2͒ in order to check for a problem with our source of
NO2. Our two data sets agree within experimental uncer-
tainty, except for the COϪ3 reaction at 500 K, i.e., for the
smallest rate constant measured for NO2 in this study. We
attribute the slightly larger rate constant observed to a small
͑ϳ1%͒ HNO3 impurity in the synthesized NO2. For an im-
purity in our sample to be the cause of the discrepancy be-
tween our results and the previous measurements, the impu-
rity must be nonreactive and make up over 80% of the
sample. ͑A fast reacting impurity will yield larger rather than
smaller rate constants.͒ This scenario seems highly unlikely.
The good agreement between the branching ratios measured
in the present and beam experiments indicates that impurities
were probably not a problem in the beam experiment either.
Likely causes for the discrepancy in rate constants are cali-
bration errors in the beam apparatus pressure measurement
or differing energy distributions.
FIG. 3. Percentage of NOϪ3 product formed in the reaction of O3Ϫ with NO2
as a function of temperature. A power law dependence of the data is shown
as a dashed line.
%NO3Ϫϭ2.3ϫ107ϫTϪ2.52
.
͑6͒
The scatter in the data is attributed to low signal levels.
The mechanism of reaction ͑5͒ is likely to involve initial
charge transfer which is then followed by an intracomplex
rearrangement. The percentage of the observed NOϪ3 product
ion increases with decreasing temperature, where the com-
plex lifetime becomes longer and more time is available for
rearrangement. The temperature dependence of the branch-
ing ratio is approximately what is expected for the tempera-
ture dependence of the complex lifetime.13
Thermal rate constants for the reactions of COϪ3 and O3Ϫ
with NO2 were measured previously at the NOAA
laboratory,3,4 and these are plotted in Fig. 2 as open points.
The agreement is not very satisfactory, only within about a
factor of 3–5 which is quite unusual. Data from our labora-
tory usually agree very well with data taken at the NOAA
laboratory, e.g., the data shown in Fig. 1 and those reported
elsewhere.7,14,15 However, the NOAA group reported NOϪ3 as
the exclusive product of the reaction of OϪ3 with NO2. At
room temperature we find that NOϪ3 accounts for only 12%
of the reactivity. The NOAA group looked specifically for
the charge transfer product, as they attempted to bracket the
electron affinity of NO2, and the fact that they observed only
NOϪ3 indicates some unknown chemistry probably interfered
in their flowing afterglow measurements, possibly from O
atoms or O3 formed in the ion source. The NOAA flowing
afterglow measurements discussed here were performed us-
ing a pure oxygen buffer gas. For this reason, we repeated
our measurements using an oxygen buffer but found no sig-
nificant difference from the data taken using a helium buffer.
A previously reported beam study16 of the reaction of
OϪ3 with NO2 also yielded a rate constant larger than the
present value and in satisfactory agreement with the NOAA
results. However, Lifschitz et al.16 found that the majority of
the reactivity is due to charge transfer, as reported in the
present study. They also found that the charge transfer con-
tribution increases with increasing collision energy. The per-
centage of NOϪ3 production found in their experiment is in
For these reasons, we recommend the following power
law expressions for the rate constants based exclusively on
the present results:
Ϫ2.38
kCO ϩNO ϭ2.6ϫ10Ϫ5
T
,
͑7͒
͑8͒
Ϫ
3
*
2
Ϫ0.79
kO ϩNO ϭ9.1ϫ10Ϫ9
T
.
Ϫ
*
2
3
An additional measurement of these rate constants is war-
ranted to help resolve the discrepancy.
Rate constants for the reactions of COϪ3 ͑H2O͒ with NO
and NO2 are shown in Fig. 4. Data from the NOAA labora-
tory are also included in the figure. As discussed previously,
these reactions were examined in the present study at tem-
peratures of р200 K only, while the NOAA workers studied
the reactions at room temperature only. ͓The NOAA re-
searchers were able to perform the experiments at room tem-
perature because water was present in the flow tube, so that
COϪ3 and CO3Ϫ͑H2O͒ were in equilibrium.͔ Our low tempera-
ture rate constant measurements for the reaction of
COϪ3 ͑H2O͒ with NO, together with the NOAA room tem-
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Arnold, Morris, and Viggiano: Reactions with NO and NO2
2457
is approximately what might be expected for the temperature
dependence of the complex lifetime.13 It is estimated that a
10% temperature variation will have a 10%–30% effect on
the rate constant. Thus, better estimates for the pertinent at-
mospheric rate constants may be obtained by applying a tem-
perature dependence to the 200 K value similar to that found
for the reaction of COϪ3 ͑H2O͒ with NO, namely TϪ2.7. Since
only small extrapolations from 200 K are needed, these two
cases, namely T0 and TϪ2.7, probably give a good bound to
the rate constant at other temperatures.
CONCLUSIONS
We have measured temperature dependencies for the rate
constants of COϪ3 , CO3Ϫ͑H2O͒, and OϪ3 reacting with NO and
NO2, except for the reaction of COϪ3 ͑H2O͒ with NO2 for
which only a 200 K rate constant was measured. The present
measurements have serious implications for the application
of reactions ͑1͒ and ͑2͒ in deriving NO and NO2 concentra-
tions in the atmosphere as discussed below.
Previous temperature dependencies of the rate constants
for the reactions of CO3Ϫ and OϪ3 with NO are in good agree-
ment with the present measurements. We found that the re-
action of COϪ3 ͑H2O͒ with NO is about a factor of 4 faster at
200 K compared with the previous 300 K measurement. This
translates into derived NO concentrations that are in error by
the same amount since the temperature of the atmosphere is
about 200 K in the region where the NO concentration mea-
surements were made.
Previous measurements of the rate constants for NO2
reacting with COϪ3 , CO3Ϫ͑H2O͒, and OϪ3 appear to be in error.
The discrepancies are large, and in all cases the previously
reported rate constant values are too high. Depending on the
reaction, errors of factors of 3–6 are found. This has impor-
tant implications for derivations of NO2 concentrations using
the published chemical ionization mass spectrometric
technique.1,2
For all these reactions, we recommend temperature de-
pendencies of the rate constants for use in atmospheric
chemistry. In all cases except the reaction of COϪ3 ͑H2O͒ with
NO2, these recommendations are based on the present mea-
surements of the rate constants as a function of temperature.
For the reaction of CO3Ϫ͑H2O͒ with NO2, we could measure
a rate constant at 200 K only, and we assume a temperature
dependence for the small extrapolation needed. This assump-
tion should lead to errors no larger than 30%.
FIG. 4. Rate constants for the reactions of COϪ3 ͑H2O͒ reacting with NO and
NO2 as a function of temperature. The present data are shown as solid
circles and squares, respectively. Previous data from the NOAA laboratory
͑Ref. 3͒ are shown as open circles and squares, respectively. A power law
dependence for the NO data is shown as a solid line.
perature measurement, fit nicely to a power law. Thus, we
recommend the following expression for the rate constant for
COϪ3 ͑H2O͒ reacting with NO:
Ϫ2.72
kCO ͑H O)ϩNOϭ4.1ϫ10Ϫ5
T
.
͑9͒
Ϫ
3
*
2
The reaction produces mainly NOϪ2 , with NO2Ϫ͑H2O͒ com-
prising less than 8% of the total product ion signal at 100 K
and a negligible amount at 200 K. In the atmosphere, an
equilibrium between NOϪ2 and NO2Ϫ͑H2O͒ is quickly estab-
lished.
No temperature dependence could be measured for the
reaction of CO3Ϫ͑H2O͒ with NO2. The CO3Ϫ͑H2O͒ ion ther-
mally dissociates at temperatures much above 200 K, and the
NO2 freezes in the inlet line at temperatures much below 200
K. The rate constant for this reaction at 196 K is 7.9ϫ10Ϫ11
cm3 sϪ1. The rate constant reported by NOAA for 300 K is
ϳ1.5ϫ10Ϫ10 cm3 sϪ1. As with the other NO2 reactions dis-
cussed previously, the NOAA rate constant for the reaction
of COϪ3 ͑H2O͒ with NO2 is significantly larger than the
present value. This is especially true when one takes into
account the expected negative temperature dependence of the
reactivity. For the same reasons stated earlier, we feel the
rate constant determined in the present study is the more
reliable value. However, we welcome another measurement
to resolve this discrepancy.
ACKNOWLEDGMENTS
The PL authors would like to thank John Williamson and
Paul Mundis for technical assistance. The work has been
supported by the Strategic Environmental Research and De-
velopment Program and the Air Force Office of Scientific
Research.
The 196 K rate constant reported here for the reaction of
COϪ3 ͑H2O͒ with NO2 is a reasonable first estimate for the
rate constants required for atmospheric measurements since
the temperature at which reaction ͑2͒ is used for trace gas
analysis in the atmosphere is approximately 200 K. How-
ever, most inefficient ion–molecule reactions have rate con-
stants that decrease with increasing temperature,17 including
those measured in the present study. Slow ion–molecule re-
actions generally have a weak negative temperature depen-
dence. For reactions like those in the present study a depen-
dence between TϪ1 and TϪ3 is reasonable. The upper range
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