In:
Energy & Environmental Science, Royal Society of Chemistry (RSC), Vol. 17, No. 10 ( 2024), p. 3594-3603
Abstract:
The selective electrochemical conversion of CO 2 /CO into valuable C 2+ oxygenates and hydrocarbons using Cu-based catalysts is regarded as a promising strategy for carbon cycle utilization. Herein, we synthesized Cu x P 2 O x +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 Cu x P 2 O x +5 cell volume. Reconstructed Cu x P 2 O x +5 shows a grain boundary-dependent performance in CO electrolysis, with a C 2+ faradaic efficiency over 90% at a current density greater than 1.0 A cm −2 . Among them, reconstructed Cu 5 P 2 O 10 , with the highest surface density of grain boundary, achieves a C 2+ current density of 1.70 A cm −2 and a C 2+ 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 H 2 O dissociation sites, which facilitate *CO–COH formation for C 2+ production.
Type of Medium:
Online Resource
ISSN:
1754-5692
,
1754-5706
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2024
detail.hit.zdb_id:
2439879-2
detail.hit.zdb_id:
2448515-9
