Issue 22, 2024

Enhancing C2+ product selectivity in CO2 electroreduction by enriching intermediates over carbon-based nanoreactors

Abstract

Electrochemical CO2 reduction reaction (CO2RR) to multicarbon (C2+) products faces challenges of unsatisfactory selectivity and stability. Guided by finite element method (FEM) simulation, a nanoreactor with cavity structure can facilitate C–C coupling by enriching *CO intermediates, thus enhancing the selectivity of C2+ products. We designed a stable carbon-based nanoreactor with cavity structure and Cu active sites. The unique geometric structure endows the carbon-based nanoreactor with a remarkable C2+ product faradaic efficiency (80.5%) and C2+-to-C1 selectivity (8.1) during the CO2 electroreduction. Furthermore, it shows that the carbon shell could efficiently stabilize and highly disperse the Cu active sites for above 20 hours of testing. A remarkable C2+ partial current density of−323 mA cm−2 was also achieved in a flow cell device. In situ Raman spectra and density functional theory (DFT) calculation studies validated that the *COatop intermediates are concentrated in the nanoreactor, which reduces the free energy of C–C coupling. This work unveiled a simple catalyst design strategy that would be applied to improve C2+ product selectivity and stability by rationalizing the geometric structures and components of catalysts.

Graphical abstract: Enhancing C2+ product selectivity in CO2 electroreduction by enriching intermediates over carbon-based nanoreactors

Supplementary files

Article information

Article type
Edge Article
Submitted
14 Mar 2024
Accepted
30 Apr 2024
First published
01 May 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2024,15, 8451-8458

Enhancing C2+ product selectivity in CO2 electroreduction by enriching intermediates over carbon-based nanoreactors

M. Wang, C. Chen, S. Jia, S. Han, X. Dong, D. Zhou, T. Yao, M. Fang, M. He, W. Xia, H. Wu and B. Han, Chem. Sci., 2024, 15, 8451 DOI: 10.1039/D4SC01735H

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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