Operando studies reveal active Cu nanograins for CO2 electroreduction

Yao Yang, Sheena Louisia, Sunmoon Yu, Jianbo Jin, Inwhan Roh, Chubai Chen, Maria V. Fonseca Guzman, Julian Feijóo, Peng-Cheng Chen, Hongsen Wang, Christopher J. Pollock, Xin Huang, Yu-Tsun Shao, Cheng Wang, David A. Muller, Héctor D. Abruña and Peidong Yang ()
Additional contact information
Yao Yang: University of California
Sheena Louisia: University of California
Sunmoon Yu: Lawrence Berkeley National Laboratory
Jianbo Jin: University of California
Inwhan Roh: University of California
Chubai Chen: University of California
Maria V. Fonseca Guzman: University of California
Julian Feijóo: University of California
Peng-Cheng Chen: University of California
Hongsen Wang: Cornell University
Christopher J. Pollock: Cornell University
Xin Huang: Cornell University
Yu-Tsun Shao: Cornell University
Cheng Wang: Lawrence Berkeley National Laboratory
David A. Muller: Cornell University
Héctor D. Abruña: Cornell University
Peidong Yang: University of California

Nature, 2023, vol. 614, issue 7947, 262-269

Abstract: Abstract Carbon dioxide electroreduction facilitates the sustainable synthesis of fuels and chemicals1. Although Cu enables CO2-to-multicarbon product (C2+) conversion, the nature of the active sites under operating conditions remains elusive2. Importantly, identifying active sites of high-performance Cu nanocatalysts necessitates nanoscale, time-resolved operando techniques3–5. Here, we present a comprehensive investigation of the structural dynamics during the life cycle of Cu nanocatalysts. A 7 nm Cu nanoparticle ensemble evolves into metallic Cu nanograins during electrolysis before complete oxidation to single-crystal Cu2O nanocubes following post-electrolysis air exposure. Operando analytical and four-dimensional electrochemical liquid-cell scanning transmission electron microscopy shows the presence of metallic Cu nanograins under CO2 reduction conditions. Correlated high-energy-resolution time-resolved X-ray spectroscopy suggests that metallic Cu, rich in nanograin boundaries, supports undercoordinated active sites for C–C coupling. Quantitative structure–activity correlation shows that a higher fraction of metallic Cu nanograins leads to higher C2+ selectivity. A 7 nm Cu nanoparticle ensemble, with a unity fraction of active Cu nanograins, exhibits sixfold higher C2+ selectivity than the 18 nm counterpart with one-third of active Cu nanograins. The correlation of multimodal operando techniques serves as a powerful platform to advance our fundamental understanding of the complex structural evolution of nanocatalysts under electrochemical conditions.

Date: 2023
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DOI: 10.1038/s41586-022-05540-0

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