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
ISSN2155-5435
卷号10期号:11页码:6346-6355
发表状态已发表
DOI10.1021/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.
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