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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 |
ISSN | 2044-4753 |
EISSN | 2044-4761 |
卷号 | 10期号:10页码:3346-3352 |
发表状态 | 已发表 |
DOI | 10.1039/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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