Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field

Weihua Guo, Siwei Zhang, Junjie Zhang, Haoran Wu, Yangbo Ma, Yun Song, Le Cheng, Liang Chang, Geng Li, Yong Liu, Guodan Wei, Lin Gan, Minghui Zhu (), Shibo Xi (), Xue Wang, Boris I. Yakobson (), Ben Zhong Tang () and Ruquan Ye ()
Additional contact information
Weihua Guo: City University of Hong Kong
Siwei Zhang: The Hong Kong University of Science and Technology
Junjie Zhang: Rice University, 6100 Main Street
Haoran Wu: East China University of Science and Technology
Yangbo Ma: City University of Hong Kong
Yun Song: City University of Hong Kong
Le Cheng: City University of Hong Kong
Liang Chang: Tsinghua Shenzhen International Graduate School, Tsinghua University
Geng Li: City University of Hong Kong
Yong Liu: City University of Hong Kong
Guodan Wei: Tsinghua Shenzhen International Graduate School, Tsinghua University
Lin Gan: Tsinghua Shenzhen International Graduate School, Tsinghua University
Minghui Zhu: East China University of Science and Technology
Shibo Xi: Institute of Chemical and Engineering Sciences, A*STAR
Xue Wang: City University of Hong Kong
Boris I. Yakobson: Rice University, 6100 Main Street
Ben Zhong Tang: The Hong Kong University of Science and Technology
Ruquan Ye: City University of Hong Kong

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Regulating electron transport rate and ion concentrations in the local microenvironment of active site can overcome the slow kinetics and unfavorable thermodynamics of CO2 electroreduction. However, simultaneous optimization of both kinetics and thermodynamics is hindered by synthetic constraints and poor mechanistic understanding. Here we leverage laser-assisted manufacturing for synthesizing CuxO bipyramids with controlled tip angles and abundant nanograins, and elucidate the mechanism of the relationship between electron transport/ion concentrations and electrocatalytic performance. Potassium/OH− adsorption tests and finite element simulations corroborate the contributions from strong electric field at the sharp tip. In situ Fourier transform infrared spectrometry and differential electrochemical mass spectrometry unveil the dynamic evolution of critical *CO/*OCCOH intermediates and product profiles, complemented with theoretical calculations that elucidate the thermodynamic contributions from improved coupling at the Cu+/Cu2+ interfaces. Through modulating the electron transport and ion concentrations, we achieve high Faradaic efficiency of 81% at ~900 mA cm−2 for C2+ products via CO2RR. Similar enhancement is also observed for nitrate reduction reaction (NITRR), achieving 81.83 mg h−1 ammonia yield rate per milligram catalyst. Coupling the CO2RR and NITRR systems demonstrates the potential for valorizing flue gases and nitrate wastes, which suggests a practical approach for carbon-nitrogen cycling.

Date: 2023
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DOI: 10.1038/s41467-023-43303-1

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