Gallium nitride catalyzed the direct hydrogenation of carbon dioxide to dimethyl ether as primary product

Chang Liu, Jincan Kang, Zheng-Qing Huang, Yong-Hong Song, Yong-Shan Xiao, Jian Song, Jia-Xin He, Chun-Ran Chang (), Han-Qing Ge, Ye Wang (), Zhao-Tie Liu and Zhong-Wen Liu ()
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Chang Liu: Shaanxi Normal University
Jincan Kang: Xiamen University
Zheng-Qing Huang: Xi’an Jiaotong University
Yong-Hong Song: Shaanxi Normal University
Yong-Shan Xiao: Shaanxi Normal University
Jian Song: Shaanxi Normal University
Jia-Xin He: Shaanxi Normal University
Chun-Ran Chang: Xi’an Jiaotong University
Han-Qing Ge: Shaanxi Normal University
Ye Wang: Xiamen University
Zhao-Tie Liu: Shaanxi Normal University
Zhong-Wen Liu: Shaanxi Normal University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The selective hydrogenation of CO2 to value-added chemicals is attractive but still challenged by the high-performance catalyst. In this work, we report that gallium nitride (GaN) catalyzes the direct hydrogenation of CO2 to dimethyl ether (DME) with a CO-free selectivity of about 80%. The activity of GaN for the hydrogenation of CO2 is much higher than that for the hydrogenation of CO although the product distribution is very similar. The steady-state and transient experimental results, spectroscopic studies, and density functional theory calculations rigorously reveal that DME is produced as the primary product via the methyl and formate intermediates, which are formed over different planes of GaN with similar activation energies. This essentially differs from the traditional DME synthesis via the methanol intermediate over a hybrid catalyst. The present work offers a different catalyst capable of the direct hydrogenation of CO2 to DME and thus enriches the chemistry for CO2 transformations.

Date: 2021
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DOI: 10.1038/s41467-021-22568-4

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