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首页> 外文期刊>RSC Advances >Effects of water, ammonia and formic acid on HO2 + Cl reactions under atmospheric conditions: competition between a stepwise route and one elementary step
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Effects of water, ammonia and formic acid on HO2 + Cl reactions under atmospheric conditions: competition between a stepwise route and one elementary step

机译：水，氨和甲酸对大气条件下HO2 + CL反应的影响：逐步途径与一个基本步骤之间的竞争

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摘要

Quantum chemical calculations at M06-2X and CCSD(T) levels of theory have been performed to investigate the effects of H2O, NH3, and HCOOH on the HO2 + Cl -> HCl + O-2 reaction. The results show that catalyzed reactions with three catalysts could proceed through two different mechanisms, namely a stepwise route and one elementary step, where the former reaction is more favorable than the latter. Meanwhile, for the stepwise route, a single hydrogen atom transfer pathway in the presence of all catalysts has more advantages than the respective double hydrogen atom transfer pathway. Then, the relative impacts of catalysts under tropospheric conditions were investigated by considering the temperature dependence of the rate constants and the altitude dependence of catalyst concentrations. The calculated results show that at 0 km altitude, the HO2 + Cl -> HCl + O-2 reaction with catalysts, such as H2O, NH3, or HCOOH, cannot compete with the reaction without a catalyst, as the effective rate constant with a catalyst is smaller by 2-6 orders of magnitude than the naked reaction within the temperature range 280-320 K. The calculated results also show that at altitudes of 5, 10 and 15 km, the effective rate constant of the HCOOH-catalyzed reaction increases obviously with an increase in altitude. At 15 km altitude, its value is up to 9.63 x 10(-11) cm(3) per molecule per s, which is close to the corresponding value of the reaction without a catalyst, showing that the contribution of HCOOH to the HO2 + Cl -> HCl + O-2 reaction cannot be neglected at high altitudes. The new findings in this investigation are not only of great necessity and importance for elucidating the gas-phase reaction of HO2 with Cl in the presence of acidic, neutral and basic catalysts, but are also of great interest for understanding the importance of other types of hydrogen abstraction in the atmosphere.
机译：已经进行了M06-2X和CCSD（T）理论水平的量子化学计算，以研究H 2 O，NH 3和HCOOH对HO2 + Cl - > HCl + O-2反应的影响。结果表明，具有三种催化剂的催化反应可以通过两种不同的机制，即逐步途径和一个基本步骤，其中前反应比后者更有利。同时，对于逐步途径，所有催化剂存在下的单个氢原子转移途径比相应的双氢原子转移途径具有更多的优点。然后，通过考虑速率常数的温度依赖性和催化剂浓度的高度依赖性，研究了催化剂在对流层条件下的相对冲击。计算结果表明，在0公里的高度，HO2 + Cl - > HCl + O-2与催化剂的反应，例如H 2 O，NH 3或HCOOH，不能与没有催化剂的反应竞争，因为具有a的有效速率常数催化剂小于温度范围内的裸反应280-320k的态度较小。计算结果还表明，在5,10和15km的海拔，HCOOH催化反应的有效率常数增加显然随着高度的增加。在15公里处，其值每分的每分子可达9.63×10（-11）厘米（3），其接近没有催化剂的反应的相应值，显示HCOOH对HO2 +的贡献Cl - > HCl + O-2反应在高海拔不忽略。本研究中的新发现不仅具有良好的必要性和重要性，可以在酸性，中性和碱性催化剂存在下阐明HO2与CL的气相反应，但对理解其他类型的重要性也很有兴趣大气中的氢气抽象。

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  • 来源
    《RSC Advances》 |2019年第37期|共13页
  • 作者

    Zhang Tianlei; Zhang Yongqi; Wen Mingjie; Tang Zhuo; Long Bo; Yu Xiaohu; Zhao Caibin; Wang Wenliang;

  • 作者单位

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Guizhou Minzu Univ Sch Mat Sci &

    Engn Guiyang 550025 Guizhou Peoples R China;

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Shaanxi Univ Technol Sch Chem &

    Environm Sci Shaanxi Key Lab Catalysis Hanzhong 723001 Shaanxi Peoples R China;

    Shaanxi Normal Univ Sch Chem &

    Chem Engn Key Lab Macromol Sci Shaanxi Prov Xian 710062 Shaanxi Peoples R China;

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