Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products

Jia，Yufei1; Ding，Yunxuan2; Song，Tao3; Xu，Yunlong1; Li，Yaqing1; Duan，Lele3; Li，Fei1; Sun，Licheng1,2; Fan，Ke1

2023

10.1002/advs.202303726

Advanced Science   Impact Factor & Quartile

2198-3844

The recognition of the surface reconstruction of the catalysts during electrochemical CO reduction (CO2RR) is essential for exploring and comprehending active sites. Although the superior performance of Cu–Zn bimetallic sites toward multicarbon C products has been established, the dynamic surface reconstruction has not been fully understood. Herein, Zn-doped CuO nano-octahedrons are used to investigate the effect of the dynamic stability by the leaching and redeposition on CO2RR. Correlative characterizations confirm the Zn leaching from Zn-doped CuO, which is redeposited at the surface of the catalysts, leading to dynamic stability and abundant Cu–Zn bimetallic sites at the surface. The reconstructed Zn-doped CuO catalysts achieve a high Faradaic efficiency (FE) of C products (77% at –1.1 V versus reversible hydrogen electrode (RHE)). Additionally, similar dynamic stability is also discovered in Al-doped CuO for CO2RR, proving its universality in amphoteric metal-doped catalysts. Mechanism analyses reveal that the OHC–CHO pathway can be the C–C coupling processes on bare CuO and Zn-doped CuO, and the introduction of Zn to Cu can efficiently lower the energy barrier for CO2RR to CH. This research provides profound insight into unraveling surface dynamic reconstruction of amphoteric metal-containing electrocatalysts and can guide rational design of the high-performance electrocatalysts for CO2RR.

amphoteric metal-doped Cu2O CO2 reduction electrocatalysis leaching redeposition

SCI

English

Others

National Key Ramp;D Program of China["2022YFA0911900","2022YFA0911904"] ; Fundamental Research Center of Artificial Photosynthesis (FReCAP) - National Natural Science Foundation of China[22088102] ; Natural Science Foundation of Liaoning Province[2021-MS-126] ; Fundamental Research Funds for the Central Universities["DUT22LK01","DUT22QN213"]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001040957600001

WILEY

2-s2.0-85166310822

Scopus

1.State Key Laboratory of Fine Chemicals,Institute of Artificial Photosynthesis,DUT-KTH Joint Education and Research Centre on Molecular Devices,Institute for Energy Science and Technology,Dalian University of Technology,Dalian,116024,China
2.Center of Artificial Photosynthesis for Solar Fuels,Department of Chemistry,School of Science,Westlake University,Hangzhou,310024,China
3.Department of Chemistry and Shenzhen Grubbs Institute,Southern University of Science and Technology,Shenzhen,518055,China

Jia，Yufei,Ding，Yunxuan,Song，Tao,et al. Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products[J]. Advanced Science,2023.

Jia，Yufei.,Ding，Yunxuan.,Song，Tao.,Xu，Yunlong.,Li，Yaqing.,...&Fan，Ke.(2023).Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products.Advanced Science.

Jia，Yufei,et al."Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products".Advanced Science (2023).