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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >Mechanistic insight into the quantitative synthesis of acetic acid by direct conversion of CH4 and CO2: An experimental and theoretical approach
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Mechanistic insight into the quantitative synthesis of acetic acid by direct conversion of CH4 and CO2: An experimental and theoretical approach

机译：通过CH4和CO2直接转化对乙酸定量合成的机械洞察：实验与理论方法

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摘要

Conversion of CH4 and CO2 into value-added products has vital environmental and economic importance. Their direct conversion to acetic acid is challenging due to their high activation energy. Hence, kinetic and mechanistic information are crucial for the carbonylation of CH4 with CO2. Regarding this, single and dual component catalysts with different combinations of ZnO-, CeO2-, and MnO2- supported montmorillonite (MMT) were prepared and characterized by XPS, Raman, and XRD. Quick solid-state NMR, TGA, and FT-IR techniques were used and Langmuir-Hinshelwood model was considered to investigate mechanistic steps involved in the conversion of CH4 and CO2 to acetic acid. The obtained mechanistic and kinetic results were also theoretically proved by density functional theory (DFT) calculations. We found that ZnO and CeO2 dual active sites preferentially adsorb the CH4 and CO2, respectively that avoid surface adsorption competition. The rate of acetic acid formation was maximum when these sites exist at appropriate concentration (Ce: 0.44 wt%, Zn: 2.20 wt%). DFT calculations elucidated that the formation of acetic acid is strongly favored on ZnO catalyst with easier migration of the adsorbed CO2 from CeO2 to the ZnO side.
机译：将CH4和CO2转化为增值产品具有重要的环境和经济意义。它们的直接转化为醋酸是挑战，因为它们的高活化能量很高。因此，动力学和机械信息对于CH 4与CO2的羰基化至关重要。关于该具有不同组合的ZnO-，CeO 2和MNO2-支持的蒙脱石（MMT）的单一和双组分催化剂，并通过XPS，拉曼和XRD表征。使用快速固态NMR，TGA和FT-IR技术，并考虑研究CH4和CO 2转化为乙酸的机械介绍。通过密度泛函理论（DFT）计算，理论上证明了所获得的机械和动力学结果。我们发现ZnO和CeO2双活性位点优先吸附CH4和CO2，避免表面吸附竞争。当这些位点以适当浓度（Ce：0.44wt％，Zn：2.20wt％）存在时，乙酸形成的速率最大。 DFT计算阐明了乙酸的形成在ZnO催化剂上强烈偏爱，其具有从CeO 2到ZnO侧的吸附的CO 2更容易迁移。

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