Water Splitting by C 60 -Supported Vanadium Single Atoms.

Autor: Hou GL; Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Celestijnenlaan 200D, 3001, Leuven, Belgium.; MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an, 710049, P. R. China., Yang T; MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an, 710049, P. R. China., Li M; MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an, 710049, P. R. China., Vanbuel J; Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Celestijnenlaan 200D, 3001, Leuven, Belgium., Lushchikova OV; Radboud University, Institute for Molecules and Materials, FELIX Laboratory, Toernooiveld 7, 6525, ED, Nijmegen, The Netherlands., Ferrari P; Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Celestijnenlaan 200D, 3001, Leuven, Belgium., Bakker JM; Radboud University, Institute for Molecules and Materials, FELIX Laboratory, Toernooiveld 7, 6525, ED, Nijmegen, The Netherlands., Janssens E; Quantum Solid-State Physics, Department of Physics and Astronomy, KU Leuven, Celestijnenlaan 200D, 3001, Leuven, Belgium.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2021 Dec 20; Vol. 60 (52), pp. 27095-27101. Date of Electronic Publication: 2021 Nov 10.
DOI: 10.1002/anie.202112398
Abstrakt: Water splitting is an important source of hydrogen, a promising future carrier for clean and renewable energy. A detailed understanding of the mechanisms of water splitting, catalyzed by supported metal atoms or nanoparticles, is essential to improve the design of efficient catalysts. Here, we report an infrared spectroscopic study of such a water splitting process, assisted by a C 60 supported vanadium atom, C 60 V + +H 2 O→C 60 VO + +H 2 . We probe both the entrance channel complex C 60 V + (H 2 O) and the end product C 60 VO + , and observe the formation of H 2 as a result from resonant infrared absorption. Density functional theory calculations exploring the detailed reaction pathway reveal that a quintet-to-triplet spin crossing facilitates the water splitting reaction by C 60 -supported V + , whereas this reaction is kinetically hindered on the isolated V + ion by a high energy barrier. The C 60 support has an important role in lowering the reaction barrier with more than 70 kJ mol -1 due to a large orbital overlap of one water hydrogen atom with one carbon atom of the C 60 support. This fundamental insight in the water splitting reaction by a C 60 -supported single vanadium atom showcases the importance of supports in single atom catalysts by modifying the reaction potential energy surface.
(© 2021 Wiley-VCH GmbH.)
Databáze: MEDLINE
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