中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 大连化学物理研究所
  3. 中国科学院大连化学物理研究所
Mechanistic Insights into Selective CO2 Conversion via RWGS on Transition Metal Phosphides: A DFT Study

文献类型：期刊论文

作者Guharoy, Utsab1,2; Reina, Tomas Ramirez1; Gu, Sai1; Cai, Qiong1
刊名JOURNAL OF PHYSICAL CHEMISTRY C
出版日期2019-09-19
卷号123期号:37页码:22918-22931
ISSN号1932-7447
DOI10.1021/acs.jpcc.9b04122
通讯作者Cai, Qiong(q.cai@surrey.ac.uk)
英文摘要Selective conversion of CO2 to CO via the reverse water gas shift TMPs (RWGS) reaction is an attractive CO2 conversion process, which may be integrated with many industrial catalytic processes such as Fischer-Tropsch synthesis to generate added value products. The development of active and cost friendly catalysts is of paramount importance. Among the available catalyst materials, transition metal phosphides (TMPs) such as MoP and Ni2P have remained unexplored in the context of the RWGS reaction. In the present work, we have employed density functional theory (DFT) to first investigate the stability and geometries of selected RWGS intermediates on the MoP (0001) surface, in comparison to the Ni2P (0001) surface. Higher adsorption energies and Bader charges are observed on MoP (0001), indicating better stability of intermediates on the MoP (0001) surface. Furthermore, mechanistic investigation using potential energy surface (PES) profiles showcased that both MoP and Ni2P were active toward RWGS reaction with the direct path (CO2* -> CO* + O*) favorable on MoP (0001), whereas the COOH-mediated path (CO2* + H* -> COOH*) favors Ni2P (0001) for product (CO and H2O) gas generation. Additionally, PES profiles of initial steps to CO activation revealed that direct CO decomposition to C* and O* is favored only on MoP (0001), while H-assisted CO activation is more favorable on Ni2P (0001) but could also occur on MoP (0001). Furthermore, our DFT calculations also ascertained the possibility of methane formation on Ni2P (0001) during the RWGS process, while MoP (0001) remained more selective toward CO generation.
WOS关键词GAS SHIFT REACTION ; CARBON-MONOXIDE ; HYDROGEN EVOLUTION ; ADSORPTION ; CATALYSTS ; MOLYBDENUM ; ACTIVATION ; SURFACE ; CARBIDE ; DISSOCIATION
资助项目Department of Chemical and Process Engineering at the University of Surrey ; EPSRC[EP/M027066/1] ; EPSRC[EP/R512904] ; EPSRC[EP/J020184/2] ; EPSRC[EP/P003354/1]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:000487349600023
出版者AMER CHEMICAL SOC
资助机构Department of Chemical and Process Engineering at the University of Surrey ; Department of Chemical and Process Engineering at the University of Surrey ; EPSRC ; EPSRC ; Department of Chemical and Process Engineering at the University of Surrey ; Department of Chemical and Process Engineering at the University of Surrey ; EPSRC ; EPSRC ; Department of Chemical and Process Engineering at the University of Surrey ; Department of Chemical and Process Engineering at the University of Surrey ; EPSRC ; EPSRC ; Department of Chemical and Process Engineering at the University of Surrey ; Department of Chemical and Process Engineering at the University of Surrey ; EPSRC ; EPSRC
源URL[http://cas-ir.dicp.ac.cn/handle/321008/172842]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Cai, Qiong
作者单位1.Univ Surrey, Fac Engn & Phys Sci, Dept Chem & Proc Engn, Guildford GU2 7XH, Surrey, England
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
推荐引用方式
GB/T 7714		 Guharoy, Utsab,Reina, Tomas Ramirez,Gu, Sai,et al. Mechanistic Insights into Selective CO2 Conversion via RWGS on Transition Metal Phosphides: A DFT Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2019,123(37):22918-22931.
APA Guharoy, Utsab,Reina, Tomas Ramirez,Gu, Sai,&Cai, Qiong.(2019).Mechanistic Insights into Selective CO2 Conversion via RWGS on Transition Metal Phosphides: A DFT Study.JOURNAL OF PHYSICAL CHEMISTRY C,123(37),22918-22931.
MLA Guharoy, Utsab,et al."Mechanistic Insights into Selective CO2 Conversion via RWGS on Transition Metal Phosphides: A DFT Study".JOURNAL OF PHYSICAL CHEMISTRY C 123.37(2019):22918-22931.

入库方式： OAI收割

来源：大连化学物理研究所

浏览0
下载0
收藏0
其他版本

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。