Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field
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Published:2023-11-15
Issue:1
Volume:14
Page:
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ISSN:2041-1723
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Container-title:Nature Communications
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language:en
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Short-container-title:Nat Commun
Author:
Guo Weihua, Zhang Siwei, Zhang Junjie, Wu Haoran, Ma Yangbo, Song Yun, Cheng Le, Chang Liang, Li Geng, Liu Yong, Wei GuodanORCID, Gan LinORCID, Zhu MinghuiORCID, Xi Shibo, Wang XueORCID, Yakobson Boris I.ORCID, Tang Ben ZhongORCID, Ye RuquanORCID
Abstract
AbstractRegulating 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.
Funder
Natural Science Foundation of Guangdong Province Hong Kong Research Grant Council Shenzhen Key Laboratory of Functional Aggregate Materials
Publisher
Springer Science and Business Media LLC
Subject
General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary
Reference53 articles.
1. Chu, S. & Majumdar, A. Opportunities and challenges for a sustainable energy future. Nature 488, 294–303 (2012). 2. Poliakoff, M., Fitzpatrick, J. M., Farren, T. R. & Anastas, P. T. Green chemistry: Science and politics of change. Science 297, 807 (2002). 3. Zimmerman, J. B., Anastas, P. T., Erythropel, H. C. & Leitner, W. Designing for a green chemistry future. Science 367, 397–400 (2020). 4. He, M., Sun, Y. & Han, B. Green carbon science: efficient carbon resource processing, utilization, and recycling towards carbon neutrality. Angew. Chem. Int. Ed. Engl. 61, e202112835 (2021). 5. Li, C. J. & Anastas, P. T. Green chemistry: present and future. Chem. Soc. Rev. 41, 1413–1414 (2012).
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