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Hybridization of molecular and graphene materials for CO2 photocatalytic reduction with selectivity control

DOI: 10.1021/jacs.1c02250 DOI Help

Authors: Bing Ma (Université de Paris) , Matías Blanco (University of Padova) , Laura Calvillo (University of Padova) , Lingjing Chen (Dongguan University of Technology) , Gui Chen (Dongguan University of Technology) , Tai-Chu Lau (University of Hong Kong) , Goran Dražić (National Institute of Chemistry, Slovenia) , Julien Bonin (Université de Paris) , Marc Robert (Institut Universitaire de France (IUF)) , Gaetano Granozzi (University of Padova)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of The American Chemical Society

State: Published (Approved)
Published: May 2021
Diamond Proposal Number(s): 25902

Abstract: 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.

Journal Keywords: Functionalization; Molecules; Catalysts; Selectivity; Irradiation

Diamond Keywords: Photocatalysis

Subject Areas: Materials, Chemistry

Instruments: B18-Core EXAFS

Added On: 30/05/2021 19:42

Discipline Tags:

Catalysis Physical Chemistry Materials Science Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)