Issue 22, 2024

Redox-active covalent organic nanosheets (CONs) as a metal-free electrocatalyst for selective CO2 electro-reduction to the liquid fuel methanol

Abstract

In essence, the utilization of renewable energy in the carbon dioxide reduction reaction (CO2RR) holds the potential to transform carbon emissions into valuable chemicals, encompassing a range of hydrocarbons and alcohols. Herein, we have implemented a redox-active triphenylamine (TPA)-based covalent organic nanosheets (CONs) as a metal-free electrocatalyst for CO2 reduction in 0.2 M phosphate buffer (pH-7.2). The reaction produced methanol as the only carbonaceous liquid product reaching a maximum faradaic efficiency (FE) of 51.6% under mild reaction conditions in aqueous medium. Moreover, the corresponding overpotential of the reaction was as low as 210 mV illustrating the superiority of this metal-free electrocatalyst. The mechanistic aspects are supported through experimental in situ RAS-IR (reflection–absorption), in situ Raman study as well as computational study. The superior performance of the electrocatalyst is believed to be due to the presence of redox-active 2-D nanosheets with exposed active sites. This work unlocks a way to produce methanol efficiently by the electrochemical reduction of CO2.

Graphical abstract: Redox-active covalent organic nanosheets (CONs) as a metal-free electrocatalyst for selective CO2 electro-reduction to the liquid fuel methanol

Supplementary files

Article information

Article type
Paper
Submitted
31 Jan 2024
Accepted
22 Apr 2024
First published
24 Apr 2024

J. Mater. Chem. A, 2024,12, 13266-13272

Redox-active covalent organic nanosheets (CONs) as a metal-free electrocatalyst for selective CO2 electro-reduction to the liquid fuel methanol

S. Barman, A. Dey, F. A. Rahimi, V. R. Bakuru, R. Jena, A. Ghosh and T. K. Maji, J. Mater. Chem. A, 2024, 12, 13266 DOI: 10.1039/D4TA00737A

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