Engineering low-coordination atoms on RhPt bimetallene for 12-electron ethanol electrooxidation

Low-coordination atoms can efficiently activate the adsorbates to facilitate electrochemical reactions characterized by slow kinetics and multi-electron transfer processes, yet achieving a high exposure ratio of low-coordinated atoms on the catalyst surface remains extremely challenging. Herein, we...

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Bibliographic Details
Published in:Energy & environmental science 2024-03, Vol.17 (6), p.2219-2227
Main Authors: Sun, Bin, Zhong, Wei, Ai, Xuan, Zhang, Chong, Li, Fu-Min, Chen, Yu
Format: Article
Language:English
Subjects:
Bimetals
Carbon dioxide
Catalysts
Chemical reactions
Coordination numbers
Electrochemistry
Electron transfer
Etching
Ethanol
Fourier transforms
Infrared reflection
Infrared spectroscopy
Intermediates
Oxidation
Ultrafines
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Summary:Low-coordination atoms can efficiently activate the adsorbates to facilitate electrochemical reactions characterized by slow kinetics and multi-electron transfer processes, yet achieving a high exposure ratio of low-coordinated atoms on the catalyst surface remains extremely challenging. Herein, we present the synthesis of a three-dimensional perforated RhPt bimetallene through an effective etching-replacement strategy, which exhibits numerous pores with an average size of approximately 1.4 nm, a rugged two-dimensional surface, and additional ultrafine RhPt nanocrystals with an average size of about 1.1 nm, revealing the virtues of abundant low-coordination atoms. RhPt bimetallene reveals outstanding activity (1.77 A mg −1 ) and remarkable selectivity for 12-electron ethanol oxidation to CO 2 , achieving 100% fuel utilization efficiency at 60 °C. In-depth investigation through in situ Fourier transform infrared reflection spectroscopy, coupled with theoretical calculations, shows that Rh-Pt bimetallic active sites with low coordination characteristic facilitate the C1 pathway and the removal of CO* intermediates for ethanol oxidation reaction. This work not only introduces an effective strategy for constructing model nanostructures with highly active low-coordination atoms, but also sheds light on the fundamental role of bimetallic active sites featuring low-coordination numbers in promoting the complete electrooxidation process. The three-dimensional perforated RhPt bimetallene achieves a high exposure ratio of low-coordinated RhPt diatomic sites, demonstrating excellent activity and remarkable selectivity for 12-electron ethanol oxidation to CO 2 .
ISSN:1754-5692
1754-5706
DOI:10.1039/d3ee04023b