Calculating the rate constant for the NH 2 -/sup> + CO ?NH2CO-/sup> ?H + NHCO reactions and thermodynamic properties of NH2CO-/sup>

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• 作者：G. A. Poskrebyshev
• 刊名：Kinetics and Catalysis
• 出版年：2015
• 出版时间：May 2015
• 年：2015
• 卷：56
• 期：3
• 页码：245-260
• 全文大小：884 KB
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• 作者单位：G. A. Poskrebyshev (1)
  
  1. Institute for Energy Problems of Chemical Physics, Russia Academy of Sciences, Moscow, 119334, Russia
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Catalysis
  Physical Chemistry
  Russian Library of Science
  
• 出版者：MAIK Nauka/Interperiodica distributed exclusively by Springer Science+Business Media LLC.
• ISSN：1608-3210

文摘

The Δ f H 298 0 (NH2CO-/sup>) = ?.6 ± 1 kJ/mol and S 298 0 = 260.6 ± 5.2 J mol? K? values have been obtained using the energies of isodesmic reactions within the CBS-Q approximation. Use of the CBS-Q, UMP2, UBHandHLYP, and UB3LYP approaches has afforded the most substantiated entropy value, S 298 0 = 258.2 ± 2.8 J mol? K?. The energetics of the NH2CO-/sup> ?NH 2 -/sup> + CO and NH2CO-/sup> ?H + NHCO reactions and their rate constants (k 1 and k 2, respectively) have been calculated using the UMP2, UBHandHLYP, and UB3LYP approaches. The rate constant values k 1, ?/sub> = 8.2 × 1010(T/298)1.18e?15/RT s?, which were obtained within the UB3LYP approach, are in closest agreement with available experimental data. The constants k 2, ?/sub> = 4.0 × 107(T/298)1.7e?49/RT s?, obtained using the UMP2 approach, are best consistent with indirect experimental evidence. The UB3LYP value of the rate constant of the NH 2 -/sup> + CO reaction at P = 1 atm and T = 304 K (k ? = 2.2 × 10?8 cm3 molecule? s?) suggests that this reaction should make a significant contribution to the removal of NH 2 -/sup> from the atmosphere under pre-abiogenesis conditions. The resulting NH2CO-/sup> adduct is a fairly stable compound capable of participating in the formation of the chemical composition of the prebiogenic atmosphere. This conclusion is supported by the small rate constant values k 1 = 3.3 × 10? s? and k 2 = 5.8 × × 10?8 s? at P = 1 atm and T = 304 K, which were calculated using the UB3LYP and UMP2 approaches. In addition, the k ? = 2.8 × 10?1 cm3 molecule? s? value (P = 1 atm) for the NHCO + H reaction, calculated using the UMP2 approach, indicates that this reaction makes an insignificant contribution to the disappearance of H atoms and to the formation of NH2CO-/sup> under the abiogenesis conditions.