In Situ Reconstruction of a Hierarchical Sn-Cu/SnOx Core/Shell Catalyst for High-Performance CO2 Electroreduction

Ke Ye; Zhiwen Zhou; Jiaqi Shao; Long Lin; Dunfeng Gao; Na Ta; Rui Si; Guoxiong Wang; Xinhe Bao

doi:10.1002/anie.201916538

In Situ Reconstruction of a Hierarchical Sn-Cu/SnO_x Core/Shell Catalyst for High-Performance CO₂ Electroreduction

Angew Chem Int Ed Engl. 2020 Mar 16;59(12):4814-4821. doi: 10.1002/anie.201916538. Epub 2020 Feb 4.

Authors

Ke Ye^{1

2}, Zhiwen Zhou^{1

3}, Jiaqi Shao^{1

2}, Long Lin^{1

3}, Dunfeng Gao¹, Na Ta¹, Rui Si⁴, Guoxiong Wang¹, Xinhe Bao¹

Affiliations

¹ State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, China.
² Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering University, Nantong Street 145, Harbin, 150001, China.
³ University of Chinese Academy of Sciences, Beijing, 100039, China.
⁴ Shanghai Synchrotron Radiation Facility, Zhangjiang Laboratory, Shanghai, 201204, China.

PMID: 31944516
DOI: 10.1002/anie.201916538

Abstract

The electrochemical CO₂ reduction reaction (CO₂ RR) to give C₁ (formate and CO) products is one of the most techno-economically achievable strategies for alleviating CO₂ emissions. Now, it is demonstrated that the SnO_x shell in Sn_2.7 Cu catalyst with a hierarchical Sn-Cu core can be reconstructed in situ under cathodic potentials of CO₂ RR. The resulting Sn_2.7 Cu catalyst achieves a high current density of 406.7±14.4 mA cm^-2 with C₁ Faradaic efficiency of 98.0±0.9 % at -0.70 V vs. RHE, and remains stable at 243.1±19.2 mA cm^-2 with a C₁ Faradaic efficiency of 99.0±0.5 % for 40 h at -0.55 V vs. RHE. DFT calculations indicate that the reconstructed Sn/SnO_x interface facilitates formic acid production by optimizing binding of the reaction intermediate HCOO* while promotes Faradaic efficiency of C₁ products by suppressing the competitive hydrogen evolution reaction, resulting in high Faradaic efficiency, current density, and stability of CO₂ RR at low overpotentials.

Keywords: carbon dioxide reduction; electrochemistry; hierarchical structures; interfaces; tin oxide.

Abstract

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