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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.
The conversion of CO2 to valuable chemicals is still challenged by catalyst developments. Herein, the authors found that GaN is an efficient catalyst for selective CO2 hydrogenation to dimethyl ether as the primary product, in contrast to the traditional methanol-intermediate route over hybrid catalysts.
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1 Shaanxi Normal University, Key Laboratory of Syngas Conversion of Shaanxi Province, School of Chemistry and Chemical Engineering, Xi’an, China (GRID:grid.412498.2) (ISNI:0000 0004 1759 8395)
2 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233)
3 Xi’an Jiaotong University, Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi’an, China (GRID:grid.43169.39) (ISNI:0000 0001 0599 1243)