CAS OpenIR  > 中科院上海应用物理研究所2011-2020年
Core-shell nanoporous AuCu3@Au monolithic electrode for efficient electrochemical CO2 reduction
Ma, XM; Shen, YL; Yao, S; An, CH; Zhang, WQ; Zhu, JF; Si, R; Guo, CX; An, CH
AbstractSelective conversion of carbon dioxide (CO2) to a reusable form of carbon via electrochemical reduction has attracted intensive interest for the storage of renewable energy. However, the achievement of efficient bulk monolithic electrocatalysts still remains a challenge. Herein, a facile oxidative etching of the Au20Cu80 alloy was developed for the synthesis of a monolithic nanoporous core-shell structured AuCu3@Au electrode, which showed a faradaic efficiency (FE) of 97.27% with a partial current density of 5.3 mA cm(-2) at -0.6 V vs. RHE for the production of CO. The FE value is about 1.45 times higher than that over the Au nanocatalyst. Unlike single nanoporous Au, AuCu3@Au maintained an excellent performance in a broad potential window. Furthermore, a 23 cm long nanoporous AuCu3@Au bulk electrode with good ductility was prepared, over which the active current reached up to 37.2 mA with a current density of 10.78 mA cm(-2) at -0.7 V vs. RHE, pushing the reduction of CO2 to industrialization. The unsaturated coordination environment with a coordination number of 8.2 over the shell gold and curved interface determined this high electrocatalytic performance. Density functional theory calculations suggested that the double-dentate adsorption structure in the AuCu3@Au catalyst effectively improves the stability of the *COOH intermediate. The density of states indicates that the introduction of Cu causes the d-band-centre of AuCu3@Au to move toward the Fermi level, directly bonding with *COOH. Therefore, the adsorption of *COOH on the surface of the AuCu3@Au catalyst is strengthened, facilitating the formation of CO. This work opens an avenue to achieve self-supported porous electrodes for various useful catalytic conversions.
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Affiliation1.Tianjin Univ Technol, Tianjin Key Lab Organ Solar Cells & Photochem Con, Inst New Energy Mat & Low Carbon Technol, Sch Chem & Chem Engn,Tianjin Key Lab Adv Funct Po, Tianjin 300384, Peoples R China
2.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
3.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
4.Suzhou Univ Sci & Technol, Inst Adv Mat & Devices, Suzhou 215009, Peoples R China
Recommended Citation
GB/T 7714
Ma, XM,Shen, YL,Yao, S,et al. Core-shell nanoporous AuCu3@Au monolithic electrode for efficient electrochemical CO2 reduction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(6):3344-3350.
APA Ma, XM.,Shen, YL.,Yao, S.,An, CH.,Zhang, WQ.,...&An, CH.(2020).Core-shell nanoporous AuCu3@Au monolithic electrode for efficient electrochemical CO2 reduction.JOURNAL OF MATERIALS CHEMISTRY A,8(6),3344-3350.
MLA Ma, XM,et al."Core-shell nanoporous AuCu3@Au monolithic electrode for efficient electrochemical CO2 reduction".JOURNAL OF MATERIALS CHEMISTRY A 8.6(2020):3344-3350.
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