First-Principles Microkinetic Study of Methanol Synthesis on Cu(221) and ZnCu(221) Surfaces |
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| Authors: | Sha-sha Wang Min-zhen Jian Hai-yan Su Wei-xue Li |
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| Affiliation: | a.State Key Laboratory of Catalysis, State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 110623, Chinab.School of Chemistry and Materials Science, Hefei National Laboratory for Physical Sciences at Microscales, University of Science and Technology of China, Hefei 230026, Chinac.University of Chinese Academy of Sciences, Beijing 100049, China |
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| Abstract: | First-principle based microkinetic simulations are performed to investigate methanol synthesis from CO and CO2 on Cu(221) and CuZn(221) surfaces. It is found that regardless of surface structure, the carbon consumption rate follows the order:CO hydrogenation > CO/CO2 hydrogenation > CO2 hydrogenation. The superior CO hydrogenation activity mainly arises from the lower barriers of elementary reactions than CO2 hydrogenation. Compared to Cu(221), the introduction of Zn greatly lowers the activity of methanol synthesis, in particularly for CO hydrogenation. For a mixed CO/CO2 hydrogenation, CO acts as the carbon source on Cu(221) while both CO and CO2 contribute to carbon conversion on CuZn(221). The degree of rate control studies show that the key steps that determine the reaction activity of CO/CO2 hydrogenation are HCO and HCOO hydrogenation on Cu(221), instead of HCOOH hydrogenation on CuZn(221). The present work highlights the effect of the Zn doping and feed gas composition on methanol synthesis. |
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| Keywords: | Methanol synthesis Cu(221) CuZn(221) Density functional theory Microkinetic simulations |
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