In situ activation of post-transition metal electrocatalysts for CO2 reduction
Shuang Yang a, Bert M. Weckhuysen a, Ward van der Stam a
a Inorganic Chemistry and Catalysis, Department of Chemistry, Utrecht University, Daltonlaan, 200, Utrecht, Netherlands
Proceedings of International Conference on Frontiers in Electrocatalytic Transformations (INTERECT22)
València, Spain, 2022 November 21st - 22nd
Organizers: Sara Barja, Nongnuch Artrith and Matthew Mayer
Poster, Ward van der Stam, 025
Publication date: 11th October 2022

Tunable (bi)metallic electrocatalysts have emerged as a viable strategy to tune the electrocatalytic CO2reduction reaction (eCO2RR) for the selective production of valuable base chemicals and fuels. For example, post-transition metal electrocatalysts, such as bismuth (Bi) and tin (Sn), have shown tremendous promise in eCO2RR to HCOOH with efficiencies approaching unity. Furthermore, combinations of post-transition metals with copper (Cu) have displayed boosted selectivity and activity for eCO2RR, but the exact reaction mechanism remains debated. It is evident that the precise identification of the active sites of the electrocatalyst under operation remains a challenge, which hinders the rational design and commercial application of advanced electrocatalysts for eCO2RR. In this contribution, the in situ activation of bismuth oxyhalide and copper-tin oxide electrocatalysts will be discussed, as characterized through detailed in situ X-ray diffraction (XRD) and Raman spectroscopy. The in situ experiments revealed that doping of post-transition metals (e.g.Sn) in oxide-derived copper electrocatalysts not only boosts the performance (near unity CO formation) through tailoring of the *CO binding strength (as confirmed by theory), but also results in prolonged stability of the electrocatalysts. Furthermore, it was found that the bismuth oxyhalide electrocatalysts were in situconverted into metallic bismuth, but the presence of the different halides (Cl, Br, I) guided the in situ facet exposure and hence the catalytic performance. Our contribution shows the power of the combination of in situX-ray characterization and Raman spectroscopy for the elucidation of the active site and reaction mechanism during eCO2RR.

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