Evidence of bifunctionality of carbons and metal atoms in catalyzed acetylene hydrochlorination

Vera Giulimondi, Andrea Ruiz-Ferrando, Georgios Giannakakis, Ivan Surin, Mikhail Agrachev, Gunnar Jeschke, Frank Krumeich, Núria López, Adam H. Clark and Javier Pérez-Ramírez ()
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Vera Giulimondi: ETH Zurich
Andrea Ruiz-Ferrando: Institute of Chemical Research of Catalonia (ICIQ-CERCA)
Georgios Giannakakis: ETH Zurich
Ivan Surin: ETH Zurich
Mikhail Agrachev: ETH Zurich
Gunnar Jeschke: ETH Zurich
Frank Krumeich: ETH Zurich
Núria López: Institute of Chemical Research of Catalonia (ICIQ-CERCA)
Adam H. Clark: Paul Scherrer Institute
Javier Pérez-Ramírez: ETH Zurich

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Carbon supports are ubiquitous components of heterogeneous catalysts for acetylene hydrochlorination to vinyl chloride, from commercial mercury-based systems to more sustainable metal single-atom alternatives. Their potential co-catalytic role has long been postulated but never unequivocally demonstrated. Herein, we evidence the bifunctionality of carbons and metal sites in the acetylene hydrochlorination catalytic cycle. Combining operando X-ray absorption spectroscopy with other spectroscopic and kinetic analyses, we monitor the structure of single metal atoms (Pt, Au, Ru) and carbon supports (activated, non-activated, and nitrogen-doped) from catalyst synthesis, using various procedures, to operation at different conditions. Metal atoms exclusively activate hydrogen chloride, while metal-neighboring sites in the support bind acetylene. Resolving the coordination environment of working metal atoms guides theoretical simulations in proposing potential binding sites for acetylene in the support and a viable reaction profile. Expanding from single-atom to ensemble catalysis, these results reinforce the importance of optimizing both metal and support components to leverage the distinct functions of each for advancing catalyst design.

Date: 2023
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DOI: 10.1038/s41467-023-41344-0

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