ShanghaiTech University Knowledge Management System
Automated Generation and Analysis of the Complex Catalytic Reaction Network of Ethanol Synthesis from Syngas on Rh(111) | |
2020-06-05 | |
发表期刊 | ACS CATALYSIS |
ISSN | 2155-5435 |
卷号 | 10期号:11页码:6346-6355 |
发表状态 | 已发表 |
DOI | 10.1021/acscatal.0c00630 |
摘要 | Reactions on the surface of catalysts are rather complex, and many possible reaction pathways and intermediates are involved. We here propose a method that is able to automatically generate a catalytic reaction network and identify the preferred reaction pathway with determined uncertainty. Taking syngas conversion to ethanol on Rh(111) as an example, a reaction network consisting of 95 elementary steps was generated. Using energies calculated with an ensemble of 2000 functionals, the occurrence frequency of different ethanol formation pathways was obtained through pruning of the reaction network with mean-field microkinetic modeling. We found that CHCO is the most important reaction intermediate for ethanol formation with the highest confidence, even at varied temperatures and pressures. The transition state of CH3CH2O hydrogenation, i.e. CH3CH2O-H, possesses the highest possibility to be rate-controlling. CO has the highest possibility to be the surface dominant species at all the temperatures and pressures considered. The method developed in the current work substantially reduces the complexity of identifying the mechanism of catalytic reactions and shows great potential in expediting future catalyst design. |
关键词 | reaction network uncertainty analysis ethanol synthesis syngas BEEF-vdW Rh |
收录类别 | SCI ; SCIE ; EI |
语种 | 英语 |
资助项目 | National Natural Science Foundation of China[91745102] |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Physical |
WOS记录号 | WOS:000538766900039 |
出版者 | AMER CHEMICAL SOC |
WOS关键词 | GRAPHITIC MESOPOROUS CARBON ; INITIO MOLECULAR-DYNAMICS ; TOTAL-ENERGY CALCULATIONS ; SYNTHESIS GAS CONVERSION ; METHANOL SYNTHESIS ; CO2 HYDROGENATION ; REACTION-MECHANISM ; RH CATALYSTS ; COMBINED DFT ; TRANSITION |
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/121737 |
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_PI研究组_黄逸凡组 |
通讯作者 | Yang, Bo |
作者单位 | 1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 2.Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, 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 | Gu, Tangjie,Wang, Baochuan,Chen, Shuyue,et al. Automated Generation and Analysis of the Complex Catalytic Reaction Network of Ethanol Synthesis from Syngas on Rh(111)[J]. ACS CATALYSIS,2020,10(11):6346-6355. |
APA | Gu, Tangjie,Wang, Baochuan,Chen, Shuyue,&Yang, Bo.(2020).Automated Generation and Analysis of the Complex Catalytic Reaction Network of Ethanol Synthesis from Syngas on Rh(111).ACS CATALYSIS,10(11),6346-6355. |
MLA | Gu, Tangjie,et al."Automated Generation and Analysis of the Complex Catalytic Reaction Network of Ethanol Synthesis from Syngas on Rh(111)".ACS CATALYSIS 10.11(2020):6346-6355. |
条目包含的文件 | ||||||
文件名称/大小 | 文献类型 | 版本类型 | 开放类型 | 使用许可 |
修改评论
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。