IS THE DEPLETION OF OZONE BY HSO AN EXOTHERMIC PROCESS
IS THE DEPLETION OF OZONE BY HSO AN EXOTHERMIC PROCESS
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HSO 消耗臭氧是放热过程吗
DOI：
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发表时间：
1994
期刊：
影响因子：
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通讯作者：
M. Yáñez
中科院分区：
文献类型：
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作者：
M. Esseffar;O. Mó;M. Yáñez
采用基于从头算分子轨道理论的Gauss-2(G2)理论程序，以及避开了该理论的加性方案的其他高级从头计算[QCISD(T)和CCSD(T)/6-311++G(3df，2pd，和QCISD(T)/6-311+G(5d2f，2p)]来估算HSO的生成热。为此，我们还提出了用五阶精确的QCISD(TQ)方法而不是通常的QCISD(T)方法来评估剩余相关效应，作为对标准G2方案的进一步改进。用不同反应过程估算的0K下亚硫酸盐的生成热为−4.2±1.3kcal/mol.最重要的结果是，HSO对臭氧的消耗被预测为轻微的吸热，而不是其他理论研究得出的结论。我们还发现，HSO比SOH更稳定，但我们的计算预测的两个异构体之间的能隙比以前报道的值要小。
The Gaussian‐2 (G2) theoretical procedure, based on ab initio molecular orbital theory, as well as other high level ab initio calculations [QCISD(T) and CCSD(T)/6–311++G(3df,2pd, and QCISD(T)/6–311+G(5d2f,2p)] which avoid the additivity scheme of this theory, are used to estimate the heat of formation of HSO. For this purpose, we propose also, as a further improvement of the standard G2 scheme, to evaluate the residual correlation effects by using the QCISD(TQ) method, which is exact in fifth order rather than the usual QCISD(T) procedure. The heat of formation of HSO at 0 K estimated using different reactive processes is −4.2±1.3 kcal/mol. The most significant consequence is that the depletion of ozone by HSO is predicted to be slightly endothermic rather than exothermic, as it has been concluded in other theoretical studies. We have also found that HSO is more stable than SOH, but the energy gap between both isomers predicted by our calculations is smaller than previous reported values.