Origin of CO2 as the main carbon source in syngas-to-methanol process over Cu: theoretical evidence from a combined DFT and microkinetic modeling study
2020-05-21
发表期刊CATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
EISSN2044-4761
卷号10期号:10页码:3346-3352
发表状态已发表
DOI10.1039/d0cy00602e
摘要

The main carbon source for methanol synthesis from syngas (CO, CO2 and H-2) has been studied experimentally for decades. In the current work, we attempt to understand the origin of such observations at a molecular level by combining density functional theory (DFT) and a microkinetic modeling approach. The energetics of elementary steps in the process of CO and CO2 hydrogenation to methanol on Cu(211) were calculated by DFT. We found that the hydrogenation of CO to methanol over Cu(211) proceeds via the reaction pathway of CO -> HCO -> CH2O -> CH3O -> CH3OH. Subsequently, microkinetic modeling was performed, taking a mixture of CO, CO2 and H-2 as the reactant, with a variable ratio between CO and CO2. The microkinetic results showed that the Cu(211) surface will have a certain coverage (around 0.083 monolayer) of spectating HCOO at the steady state. More importantly, the formation rate of methanol will increase dramatically with a small amount of CO2 added to the mixture of CO and H-2 over the surface with spectating HCOO, which is in good agreement with previous experimental results. In addition, we found that the formation of methanol from CO2 hydrogenation is always faster than that from CO hydrogenation, which further supports the conclusion that the main carbon source in the syngas-to-methanol process over Cu catalyst is CO2, rather than CO.

收录类别SCI ; SCIE ; EI
资助项目National Natural Science Foundation of China[91745102] ; Shanghai Pujiang Program[16PJ1406800] ; Shanghai Young Eastern Scholar Program[QD2016049]
WOS研究方向Chemistry
WOS类目Chemistry, Physical
WOS记录号WOS:000538156300017
出版者ROYAL SOC CHEMISTRY
WOS关键词TOTAL-ENERGY CALCULATIONS ; PD-BASED CATALYSTS ; ACETYLENE HYDROGENATION ; SURFACES ; CU(111) ; FORMATE ; SELECTIVITY ; MECHANISM ; MIXTURES ; KINETICS
原始文献类型Article
引用统计
文献类型期刊论文
条目标识符https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/119310
专题物质科学与技术学院_硕士生
物质科学与技术学院_PI研究组_杨波组
物质科学与技术学院_博士生
通讯作者Yang, Bo
作者单位
1.ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
第一作者单位物质科学与技术学院
通讯作者单位物质科学与技术学院
第一作者的第一单位物质科学与技术学院
推荐引用方式
GB/T 7714
Xu, Dongyang,Wu, Panpan,Yang, Bo. Origin of CO2 as the main carbon source in syngas-to-methanol process over Cu: theoretical evidence from a combined DFT and microkinetic modeling study[J]. CATALYSIS SCIENCE & TECHNOLOGY,2020,10(10):3346-3352.
APA Xu, Dongyang,Wu, Panpan,&Yang, Bo.(2020).Origin of CO2 as the main carbon source in syngas-to-methanol process over Cu: theoretical evidence from a combined DFT and microkinetic modeling study.CATALYSIS SCIENCE & TECHNOLOGY,10(10),3346-3352.
MLA Xu, Dongyang,et al."Origin of CO2 as the main carbon source in syngas-to-methanol process over Cu: theoretical evidence from a combined DFT and microkinetic modeling study".CATALYSIS SCIENCE & TECHNOLOGY 10.10(2020):3346-3352.
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