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Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts
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Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts
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Journal Article
Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts
2023
Overview
Atomic-level coordination engineering is an efficient strategy for tuning the catalytic performance of single-atom catalysts (SACs). However, their rational design has so far been plagued by the lack of a universal correlation between the coordination symmetry and catalytic properties. Herein, we synthesised planar-symmetry-broken CuN
3
(PSB-CuN
3
) SACs through microwave heating for electrocatalytic CO
2
reduction. Remarkably, the as-prepared catalysts exhibited a selectivity of 94.3% towards formate at −0.73 V vs. RHE, surpassing the symmetrical CuN
4
catalyst (72.4% at −0.93 V vs. RHE). In a flow cell equipped with a PSB-CuN
3
electrode, over 90% formate selectivity was maintained at an average current density of 94.4 mA cm
−2
during 100 h operation. By combining definitive structural identification with operando X-ray spectroscopy and theoretical calculations, we revealed that the intrinsic local symmetry breaking from planar
D
4
h
configuration induces an unconventional
dsp
hybridisation, and thus a strong correlation between the catalytic activity and microenvironment of metal centre (i.e., coordination number and distortion), with high preference for formate production in CuN
3
moiety. The finding opens an avenue for designing efficient SACs with specific local symmetries for selective electrocatalysis.
Atomic-level coordination influences the properties of single-atom-catalysts but is difficult to precisely engineer. Here, authors study the role of local symmetry manipulation, finding planar-symmetry-broken CuN
3
catalysts outperform highly symmetrical CuN
4
for CO
2
electroreduction to formic acid.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
