Determining Structure-Activity Relationships in Oxide Derived CuSn Catalysts During CO2 Electroreduction Using X-Ray Spectroscopy

Pardo Pérez, Laura C. and Arndt, Alexander and Stojkovikj, Sasho and Ahmet, Ibbi Y. and Arens, Joshua T. and Dattila, Federico and Wendt, Robert and Guilherme Buzanich, Ana and Radtke, Martin and Davies, Veronica and Höflich, Katja and Köhnen, Eike and Tockhorn, Philipp and Golnak, Ronny and Xiao, Jie and Schuck, Götz and Wollgarten, Markus and López, Núria and Mayer, Matthew T. (2021) Determining Structure-Activity Relationships in Oxide Derived CuSn Catalysts During CO2 Electroreduction Using X-Ray Spectroscopy. Advanced Energy Materials, 12 (210332). ISSN 1614-6840

Text Determining Structure‐Activity Relationships in Oxide Derived CuSn Catalysts During CO2 Electroredu.pdf - Published Version Download (1MB)

Abstract

The development of earth-abundant catalysts for selective electrochemical CO2 conversion is a central challenge. CuSn bimetallic catalysts can yield selective CO2 reduction toward either CO or formate. This study presents oxide-derived CuSn catalysts tunable for either product and seeks to under-stand the synergetic effects between Cu and Sn causing these selectivity trends. The materials undergo significant transformations under CO2 reduc-tion conditions, and their dynamic bulk and surface structures are revealed by correlating observations from multiple methods—X-ray absorption spectros-copy for in situ study, and quasi in situ X-ray photoelectron spectroscopy for surface sensitivity. For both types of catalysts, Cu transforms to metallic Cu0under reaction conditions. However, the Sn speciation and content differ significantly between the catalyst types: the CO-selective catalysts exhibit a surface Sn content of 13 at. % predominantly present as oxidized Sn, while the formate-selective catalysts display an Sn content of ≈70 at. % consisting of both metallic Sn0 and Sn oxide species. Density functional theory simula-tions suggest that Snδ+ sites weaken CO adsorption, thereby enhancing CO selectivity, while Sn0 sites hinder H adsorption and promote formate produc-tion. This study reveals the complex dependence of catalyst structure, compo-sition, and speciation with electrochemical bias in bimetallic Cu catalysts.

Item Type:	Article
Impact Factor Value:	27.8
Subjects:	Engineering and Technology > Chemical engineering Natural sciences > Chemical sciences Natural sciences > Earth and related environmental sciences Engineering and Technology > Environmental engineering Engineering and Technology > Materials engineering Engineering and Technology > Nano-technology Natural sciences > Other natural sciences
Divisions:	Faculty of Technology
Depositing User:	Saso Stojkovik
Date Deposited:	27 Feb 2024 11:53
Last Modified:	27 Feb 2024 11:53
URI:	https://eprints.ugd.edu.mk/id/eprint/33771

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