Axial Modification of Cobalt Complexes on Heterogeneous Surface with Enhanced Electron Transfer for Carbon Dioxide Reduction

Wang, Jiong1; Huang, Xiang2; Xi, Shibo3; Xu, Hu2; Wang, Xin1

2020-08-17

10.1002/anie.202008759

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Efficient electron communication between molecular catalyst and support is critical for heterogeneous molecular electrocatalysis and yet it is often overlooked during the catalyst design. Taking CO(2)electro-reduction on tetraphenylporphyrin cobalt (PCo) immobilized onto graphene as an example, we demonstrate that adding a relay molecule improves the interfacial electron communication. While the directly immobilized PCo on graphene exhibits relatively poor electron communications, it is found that diphenyl sulfide serves as an axial ligand for PCo and it improves the redox activity of PCo on the graphene surface to facilitate the generation of [PCo](.)- active sites for CO(2)reduction. Thus, the turnover frequencies of the immobilized Co complexes are increased. Systematic structural analysis indicates that the benzene rings of diphenyl sulfide exhibit strong face-to-face stacking with graphene, which is proposed as an efficient medium to facilitate the interfacial electron communication.

axial coordination carbon dioxide reduction catalytic mechanism heterogeneous molecular electrocatalysis interfacial electron transfer

SCI ; EI

英语

NI论文

其他

academic research fund AcRF tier 1, Ministry of Education, Singapore[M4012076 RG118/18]

Chemistry

Chemistry, Multidisciplinary

WOS:000559991100001

WILEY-V C H VERLAG GMBH

20203409068336

Catalysts ; Electrocatalysis ; Electron transitions ; Redox reactions ; Pollution control ; Sulfur compounds ; Coordination reactions ; Carbon dioxide ; Cobalt deposits ; Molecules ; Graphene ; Reduction

Heavy Metal Mines:504.3 ; Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Nanotechnology:761 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

CHEMISTRY

Web of Science

1.Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore
2.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
3.Agcy Sci Technol & Res, Inst Chem & Engn Sci, Singapore 627833, Singapore

Wang, Jiong,Huang, Xiang,Xi, Shibo,et al. Axial Modification of Cobalt Complexes on Heterogeneous Surface with Enhanced Electron Transfer for Carbon Dioxide Reduction[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59:19162-19167.

Wang, Jiong,Huang, Xiang,Xi, Shibo,Xu, Hu,&Wang, Xin.(2020).Axial Modification of Cobalt Complexes on Heterogeneous Surface with Enhanced Electron Transfer for Carbon Dioxide Reduction.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59,19162-19167.

Wang, Jiong,et al."Axial Modification of Cobalt Complexes on Heterogeneous Surface with Enhanced Electron Transfer for Carbon Dioxide Reduction".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59(2020):19162-19167.