• 文献标题:   Hybridization of Molecular and Graphene Materials for CO2 Photocatalytic Reduction with Selectivity Control
  • 文献类型:   Article
  • 作  者:   MA B, BLANCO M, CALVILLO L, CHEN LJ, CHEN G, LAU TC, DRAZIC G, BONIN J, ROBERT M, GRANOZZI G
  • 作者关键词:  
  • 出版物名称:   JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
  • ISSN:   0002-7863 EI 1520-5126
  • 通讯作者地址:  
  • 被引频次:   37
  • DOI:   10.1021/jacs.1c02250 EA MAY 2021
  • 出版年:   2021

▎ 摘  要

In the quest for designing efficient and stable photocatalytic materials for CO2 reduction, hybridizing a selective noble-metal-free molecular catalyst and carbon-based light-absorbing materials has recently emerged as a fruitful approach. In this work, we report about Co quaterpyridine complexes covalently linked to graphene surfaces functionalized by carboxylic acid groups. The nanostructured materials were characterized by X-ray photoemission spectroscopy, X-ray absorption spectroscopy, IR and Raman spectroscopies, high-resolution transmission electron microscopy and proved to be highly active in the visible-light-driven CO2 catalytic conversion in acetonitrile solutions. Exceptional stabilities (over 200 h of irradiation) were obtained without compromising the selective conversion of CO2 to products (>97%). Most importantly, complete selectivity control could be obtained upon adjusting the experimental conditions: production of CO as the only product was achieved when using a weak acid (phenol or trifluoroethanol) as a co-substrate, while formate was exclusively obtained in solutions of mixed acetonitrile and triethanolamine.