Yankun Chen, Chaoyu Hao, Sai Liu, Yongen Li, Wangrui Yang, Jianwei Gao, Lifan Jiao, Jiaji Qi
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Abstract
Ventilation air methane (VAM) is one of the main greenhouse gas sources. Owing to the characteristics of low concentration of ventilation air methane and high moisture content, we build an experimental platform and take the oxidative combustion temperature and methane conversion rate as the research indexes, and the systematic research finds that the inhibitory effect of moisture on the oxidative combustion of ultra-low concentration of methane (<1%) is a nonlinear polynomial law. In the meantime, we constructed OH(H2 O)n +CH4 and studied its reaction potential energy surface using quantum chemical calculations, which used the most significant primitive reaction of methane combustion, OH+CH4 →H2 O+CH3 , as the theoretical basis. We found that as moisture content increased, so did its reaction energy barrier, making the reactants more stable, strengthening the three-body collision effect, and reducing the number of free radicals, all of which hindered the methane chain reaction. The study aimed to validate the experimental finding that moisture inhibits the oxidative combustion of ventilation air methane by examining the internal mechanism of methane oxidation. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.
水分对通风甲烷氧化燃烧影响规律的研究
通风甲烷(VAM)是主要的温室气体源之一。针对通风空气甲烷浓度低、含水率高的特点,搭建实验平台,以氧化燃烧温度和甲烷转化率为研究指标,系统研究发现,含水率对超低浓度甲烷(<1%)氧化燃烧的抑制作用为非线性多项式规律。同时,我们以OH+CH4→H2O+CH3这一甲烷燃烧过程中最重要的原始反应为理论基础,构建了OH(H2O)n+CH4并利用量子化学计算研究了其反应势能面。我们发现,随着含水率的增加,其反应能垒也随之增加,使得反应物更加稳定,三体碰撞效应增强,自由基数量减少,这些都阻碍了甲烷链反应。本研究旨在通过考察甲烷氧化的内在机理,验证水分抑制通风空气甲烷氧化燃烧的实验发现。©2024化学工业协会和John Wiley &;儿子,有限公司
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