Details

Autor(en) / Beteiligte

• Tan, Yesen
• Sun, Guilin
• Jiang, Tingting
• Liu, Dong
• Li, Qinzhen
• Yang, Sha
• Chai, Jinsong
• Gao, Shan
• Yu, Haizhu
• Zhu, Manzhou

Titel

Symmetry Breaking Enhancing the Activity of Electrocatalytic CO2 Reduction on an Icosahedron‐Kernel Cluster by Cu Atoms Regulation

Ist Teil von

• Angewandte Chemie, 2024-01, Vol.136 (4), p.n/a

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2024

Quelle

Wiley-Blackwell Journals

Beschreibungen/Notizen

• Recently, CO2 hydrogenation had a new breakthrough resulting from the design of catalysts to effectively activate linear CO2 with symmetry‐breaking sites. However, understanding the relationship between symmetry‐breaking sites and catalytic activity at the atomic level is still a great challenge. In this study, a set of gold‐copper alloy Au13Cux (x=0–4) nanoclusters were used as research objects to show the symmetry‐controlled breaking structure on the surface of nanoclusters with the help of manipulability of the Cu atoms. Among them, Au13Cu3 nanocluster displays the highest degree of symmetry‐breaking on its crystal structure compared with the other nanoclusters in the family. Where the three copper atoms occupying the surface of the icosahedral kernel unevenly with one copper atom is coordinately unsaturated (CuS2 motif relative to CuS3 motif). As expected, Au13Cu3 has an excellent hydrogenation activity of CO2, in which the current density is as high as 70 mA cm−2 (−0.97 V) and the maximum FECO reaches 99 % at −0.58 V. Through the combination of crystal structures and theoretical calculations, the excellent catalytic activity of Au13Cu3 is revealed to be indeed closely related to its asymmetric structure. Based on the Au13Cux family, the effects of the controllable structure symmetry‐breaking on the activity of CO2 reduction were investigated. Importantly, the most efficient clustered catalysts for CO2 reduction to date were prepared in this family. This work opens the way for the design of efficient CO2 reduction catalyst and the controlled tailoring of the catalytic active sites.