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CO2 Reforming of Ethanol: Density Functional Theory Calculations, Microkinetic Modeling, and Experimental Studies
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-12 , DOI: 10.1021/acscatal.9b05231 Jia Zhang 1 , Yu Mao 2 , Junshe Zhang 3 , Junfu Tian 4 , Michael B. Sullivan 1 , X.-M. Cao 5 , Yingzhi Zeng 1 , Fanxing Li 6 , P. Hu 2
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-12 , DOI: 10.1021/acscatal.9b05231 Jia Zhang 1 , Yu Mao 2 , Junshe Zhang 3 , Junfu Tian 4 , Michael B. Sullivan 1 , X.-M. Cao 5 , Yingzhi Zeng 1 , Fanxing Li 6 , P. Hu 2
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Ethanol dry reformation (EDR) is a chemical process for syngas production, which consumes a greenhouse gas and reduces carbon footprint. We present a mechanistic study of EDR over Rh catalyst based on density functional theory (DFT) calculations and microkinetic analysis. Our results show that both the initial decomposition of C2H5OH and the later C–O bond formation are crucial steps on the reaction free energy landscape. The microkinetic model suggests that the α-dehydrogenation of ethanol is the rate-determining step, and the calculated reaction rate (rH2) is 8.23 × 103 s–1. Moreover, factors behind catalyst deactivation were investigated and potential solutions were explored from both theoretical and experimental aspects. The results indicate that additional H2 could potentially mitigate catalyst deactivation by methanation of coke deposited on the catalyst. These computational and experimental efforts further the understanding of the complicated catalytic process and inspire the rational design of EDR catalysts.
中文翻译：
乙醇的CO 2重整：密度泛函理论计算，微动力学建模和实验研究
乙醇干法重整（EDR）是生产合成气的化学过程，它消耗温室气体并减少碳足迹。我们提出了基于密度泛函理论（DFT）计算和微动力学分析的Rh催化剂上EDR的机理研究。我们的结果表明，C 2 H 5 OH的初始分解和后期C–O键的形成都是反应自由能格局中的关键步骤。微观动力学模型表明，乙醇的α-脱氢是速率的决定步骤，计算出的反应速率（r H 2）为8.23×10 3 s –1。此外，研究了催化剂失活的因素，并从理论和实验两个方面探索了潜在的解决方案。结果表明，额外的H 2可能通过沉积在催化剂上的焦炭甲烷化而潜在地减轻催化剂失活。这些计算和实验工作进一步加深了对复杂催化过程的理解，并激发了EDR催化剂的合理设计。
更新日期：2020-08-21
中文翻译：
乙醇的CO 2重整：密度泛函理论计算，微动力学建模和实验研究
乙醇干法重整（EDR）是生产合成气的化学过程，它消耗温室气体并减少碳足迹。我们提出了基于密度泛函理论（DFT）计算和微动力学分析的Rh催化剂上EDR的机理研究。我们的结果表明，C 2 H 5 OH的初始分解和后期C–O键的形成都是反应自由能格局中的关键步骤。微观动力学模型表明，乙醇的α-脱氢是速率的决定步骤，计算出的反应速率（r H 2）为8.23×10 3 s –1。此外，研究了催化剂失活的因素，并从理论和实验两个方面探索了潜在的解决方案。结果表明，额外的H 2可能通过沉积在催化剂上的焦炭甲烷化而潜在地减轻催化剂失活。这些计算和实验工作进一步加深了对复杂催化过程的理解，并激发了EDR催化剂的合理设计。
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