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在 294K 时甲醇与 OH 之间反应的水催化作用及大气影响。

Water Catalysis of the Reaction between Methanol and OH at 294 K and the Atmospheric Implications.

机构信息

INFIQC (CONICET-UNC). Dpto. de Fisicoquímica-, Facultad de Ciencias Químicas-, Centro Láser de Ciencias Moleculares-, Universidad Nacional de Córdoba, Ciudad Universitaria, X5000HUA, Córdoba, Argentina.

出版信息

Angew Chem Int Ed Engl. 2017 Feb 13;56(8):2166-2170. doi: 10.1002/anie.201612151. Epub 2017 Jan 12.

DOI:10.1002/anie.201612151
PMID:28079951
Abstract

The rate coefficient for the reaction CH OH+OH was determined by means of a relative method in a simulation chamber under quasi-real atmospheric conditions (294 K, 1 atm of air) and variable humidity or water concentration. Under these conditions, a quadratic dependence of the rate coefficient for the reaction CH OH+OH on the water concentration was found. Thus the catalytic effect of water is not only important at low temperatures, but also at room temperature. The detailed mechanism responsible of the reaction acceleration is still unknown. However, this dependence should be included in the atmospheric global models since it is expected to be important in humid regions as in the tropics. Additionally, it could explain several differences regarding the global and local atmospheric concentration of methanol in tropical areas, for which many speculations about the sinks and sources of methanol have been reported.

摘要

甲醇和氢氧自由基(OH)的反应速率系数是在模拟室内的准大气条件下(294K,1 个大气压的空气)通过相对方法确定的,并可调节湿度或水浓度。在这些条件下,发现甲醇和氢氧自由基的反应速率系数与水浓度呈二次函数关系。因此,水的催化作用不仅在低温下很重要,在室温下也是如此。导致反应加速的详细机制尚不清楚。然而,由于预计在热带等潮湿地区很重要,因此这种依赖性应包含在大气全球模型中。此外,它可以解释关于热带地区甲醇的全球和局部大气浓度的几个差异,对于这些差异,已经报道了许多关于甲醇汇和源的推测。

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