Homolytic H2 dissociation for enhanced hydrogenation catalysis on oxides

Chengsheng Yang, Sicong Ma (), Yongmei Liu, Lihua Wang, Desheng Yuan, Wei-Peng Shao, Lunjia Zhang, Fan Yang, Tiejun Lin, Hongxin Ding, Heyong He, Zhi-Pan Liu, Yong Cao, Yifeng Zhu () and Xinhe Bao ()
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Chengsheng Yang: Fudan University
Sicong Ma: Chinese Academy of Sciences
Yongmei Liu: Fudan University
Lihua Wang: Chinese Academy of Sciences
Desheng Yuan: Fudan University
Wei-Peng Shao: Shanghai Tech University
Lunjia Zhang: Shanghai Tech University
Fan Yang: Shanghai Tech University
Tiejun Lin: Chinese Academy of Sciences
Hongxin Ding: Fudan University
Heyong He: Fudan University
Zhi-Pan Liu: Fudan University
Yong Cao: Fudan University
Yifeng Zhu: Fudan University
Xinhe Bao: Fudan University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract The limited surface coverage and activity of active hydrides on oxide surfaces pose challenges for efficient hydrogenation reactions. Herein, we quantitatively distinguish the long-puzzling homolytic dissociation of hydrogen from the heterolytic pathway on Ga2O3, that is useful for enhancing hydrogenation ability of oxides. By combining transient kinetic analysis with infrared and mass spectroscopies, we identify the catalytic role of coordinatively unsaturated Ga3+ in homolytic H2 dissociation, which is formed in-situ during the initial heterolytic dissociation. This site facilitates easy hydrogen dissociation at low temperatures, resulting in a high hydride coverage on Ga2O3 (H/surface Ga3+ ratio of 1.6 and H/OH ratio of 5.6). The effectiveness of homolytic dissociation is governed by the Ga-Ga distance, which is strongly influenced by the initial coordination of Ga3+. Consequently, by tuning the coordination of active Ga3+ species as well as the coverage and activity of hydrides, we achieve enhanced hydrogenation of CO2 to CO, methanol or light olefins by 4-6 times.

Date: 2024
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DOI: 10.1038/s41467-024-44711-7

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