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Amination strategy to boost the CO2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level

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Abstract

Although the Faraday efficiency (FE) for CO production of single-atom catalysts immobilized on nitrogen-doped carbon supports (M–N/C) for the CO2 electrocatalytic reduction reaction (CO2RR) is generally over 90%, M–N/C catalysts demonstrate a poor reaction current density, which is much worse than the current density at the industrial level. Herein, we first report a generalized amination strategy to significantly increase the current density for CO production of M–N/C catalysts (M = Ni, Fe, Zn). Among them, the aminated Ni single-atom catalyst achieves a remarkable CO partial current density of 450 mA cm−2 (a total current density over 500 mA cm−2) with a nearly 90% CO FE at a moderate overpotential of 0.89 V, and particularly CO FE can be maintained over 85% in a wide operating potential range from −0.5 V to −1.0 V. DFT calculations and experimental research demonstrate that the superior activity is attributed to enhanced adsorption energies of CO2* and COOH* intermediates caused by the regulation of the electronic structure of the aminated catalysts. This work provides an ingenious method for significantly increasing the current density at the industrially-relevant level of single-atom catalysts for the CO2RR.

Graphical abstract: Amination strategy to boost the CO2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level

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Supplementary files

Article information


Submitted
29 Dec 2020
Accepted
11 Feb 2021
First published
12 Feb 2021

Energy Environ. Sci., 2021, Advance Article
Article type
Paper

Amination strategy to boost the CO2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level

Z. Chen, X. Zhang, W. Liu, M. Jiao, K. Mou, X. Zhang and L. Liu, Energy Environ. Sci., 2021, Advance Article , DOI: 10.1039/D0EE04052E

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