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

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Author(s)

  • Jiong Wang
  • Xiang Huang
  • Shibo Xi
  • Hu Xu
  • Xin Wang

Detail(s)

Original languageEnglish
Pages (from-to)19162-19167
Journal / PublicationAngewandte Chemie - International Edition
Volume59
Issue number43
Online published9 Jul 2020
Publication statusPublished - 19 Oct 2020
Externally publishedYes

Abstract

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 CO2 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 CO2 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. © 2020 Wiley-VCH GmbH

Research Area(s)

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

Citation Format(s)