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Multi-twinned gold nanoparticles with tensile surface steps for efficient electrocatalytic CO2 reduction

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Abstract

CO2 reduction reactions (CO2RR) powered by renewable electricity can directly convert CO2 to hydrocarbons and fix the intermittent sustainable energy in portable chemical fuels. It is of great importance to develop advanced catalysts that can boost CO2RR with high activity, selectivity, and efficiency at low overpotentials. Here, we report the solution synthesis using H2O2 to modify the surface structures of gold multi-twinned nanoparticles (AuMPs) and create tensile surface steps. Calculations predicted significantly enhanced CO2 adsorption and boosted CO2RR capabilities with inhibited hydrogen evolution reaction activity for the tensile surface steps with modified electronic structure. The H2O2-treated AuMPs with surface steps and 3.83% tensile lattices showed much higher activity and selectivity at lower overpotentials for CO2RR than pristine gold nanoparticles. The CO-production current density reached about 98 mA cm−2 with a Faradaic efficiency of 95.7% at −0.30 V versus reversible hydrogen electrode in the flow cell, showing a half-cell energy efficiency as high as ∼83%. Our strategy represents a rational catalyst design by engineering the surface structures of metal nanoparticles and may find more applicability in future electrocatalysis.

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Acknowledgements

We thank the Analytical and Testing Center of BIT for technical support. We acknowledge the financial support from the National Natural Science Foundation of China (21971012, 21922502, and 21971017), the National Key Research and Development Program of China (2020YFB1506300), the Beijing Municipal Natural Science Foundation (JQ20007), and the Beijing Institute of Technology Research Fund Program.

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Authors and Affiliations

  1. Ministry of Education Key Laboratory of Cluster Science, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Advanced Technology Research Institute (Jinan), School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 100081, China

    Li-Wei Chen, Yu-Chen Hao, Jiani Li, Linyu Hu, Shuai Li, Di Liu, Zhejiaji Zhu, Si-Qian Wu, Hui-Zi Huang, An-Xiang Yin & Bo Wang

  2. Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China

    Yu Guo & Ya-Wen Zhang

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  1. Li-Wei Chen
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Correspondence to An-Xiang Yin.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Chen, LW., Hao, YC., Li, J. et al. Multi-twinned gold nanoparticles with tensile surface steps for efficient electrocatalytic CO2 reduction. Sci. China Chem. 65, 2188–2196 (2022). https://doi.org/10.1007/s11426-022-1315-x

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