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Homolytic H 2 dissociation for enhanced hydrogenation catalysis on oxides.

Chengsheng YangSicong MaYongmei LiuLihua WangDesheng YuanWei-Peng ShaoLunjia ZhangFan YangTiejun LinHongxin DingHeyong HeZhi-Pan LiuYong CaoYifeng ZhuXinhe Bao
Published in: Nature communications (2024)
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 Ga 2 O 3 , 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 Ga 3+ in homolytic H 2 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 Ga 2 O 3 (H/surface Ga 3+ 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 Ga 3+ . Consequently, by tuning the coordination of active Ga 3+ species as well as the coverage and activity of hydrides, we achieve enhanced hydrogenation of CO 2 to CO, methanol or light olefins by 4-6 times.
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