Issue 10, 2024

Grain boundary generation via steering CuxP2Ox+5 precursor composition enhances CO electrolysis

Abstract

The selective electrochemical conversion of CO2/CO into valuable C2+ oxygenates and hydrocarbons using Cu-based catalysts is regarded as a promising strategy for carbon cycle utilization. Herein, we synthesized CuxP2Ox+5 (x = 2, 4, and 5) by introducing phosphorous in cupric oxide, which is electrochemically reconstructed into metallic Cu in situ with a highly porous structure during CO electrolysis. Physicochemical characterizations demonstrate various degrees of grain boundary generation, which depends on the Cu atom density in the CuxP2Ox+5 cell volume. Reconstructed CuxP2Ox+5 shows a grain boundary-dependent performance in CO electrolysis, with a C2+ faradaic efficiency over 90% at a current density greater than 1.0 A cm−2. Among them, reconstructed Cu5P2O10, with the highest surface density of grain boundary, achieves a C2+ current density of 1.70 A cm−2 and a C2+ formation rate of 575.8 μmol min−1. Operando Raman spectra reveal strong CO adsorption with dominant configurations of atop and bridge. Density functional theory calculations indicate that grain boundary provides active C–C coupling and H2O dissociation sites, which facilitate *CO–COH formation for C2+ production.

Graphical abstract: Grain boundary generation via steering CuxP2Ox+5 precursor composition enhances CO electrolysis

Supplementary files

Article information

Article type
Paper
Submitted
20 Mar 2024
Accepted
12 Apr 2024
First published
17 Apr 2024

Energy Environ. Sci., 2024,17, 3594-3603

Grain boundary generation via steering CuxP2Ox+5 precursor composition enhances CO electrolysis

J. Sang, T. Liu, P. Wei, H. Li, C. Liu, Y. Wang, Y. Rong, Q. Wang, G. Wang and X. Bao, Energy Environ. Sci., 2024, 17, 3594 DOI: 10.1039/D4EE01258E

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