软模板法诱导Cu/Al2O3深孔道结构促进等离子催化CO2加氢制二甲醚

doi:10.1016/j.actphy.2025.100054

Abstract

Abstract:

Plasma-activated heterogeneous catalysis is a promising strategy for catalytic CO₂ hydrogenation under mild conditions. In this study, pore structures with deep pore channels were constructed on Al₂O₃-x via a soft template method, and Cu/Al₂O₃-x was prepared by an impregnation method, with Al₂O₃-x serving as the support for plasma-catalyzed CO₂ hydrogenation to dimethyl ether (DME). Cu/Al₂O₃-0.75/HZSM-5 demonstrated a high performance and discharge efficiency for plasma-catalyzed CO₂ hydrogenation. The CO₂ conversion and DME yield for plasma-catalyzed CO₂ hydrogenation on Cu/Al₂O₃-0.75/HZSM-5 reached 21.98% and 9.83%, respectively, with selectivities for CO, CH₃OH, and DME on Cu/Al₂O₃-0.75/HZSM-5 of 25.39%, 29.89%, and 44.72%, respectively. The deep pore structures on Al₂O₃-x serve as Cu loading sites, and the confinement effect of the pores enhances the metal-support interaction and Cu metal dispersion. More abundant and stronger Brønsted basic and Lewis acidic sites facilitate the activation and hydrogenation of CO₂. Notably, the electric field formed by Cu sites anchored in the deep pore channel structures is conducive to guiding the activated plasma CO₂ intermediates into the difficult-to-access pores for hydrogenation. Hydrogenation of the plasma-activated CO₂ intermediates in the deep pore channels is crucial for improving plasma-catalyzed CO₂ hydrogenation to DME.

Key words: Plasma catalysis, CO₂ hydrogenation, Dimethyl ether, Al₂O₃, Pore channel

Liuyun Chen, Wenju Wang, Tairong Lu, Xuan Luo, Xinling Xie, Kelin Huang, Shanli Qin, Tongming Su, Zuzeng Qin, Hongbing Ji. Soft template-induced deep pore structure of Cu/Al₂O₃ for promoting plasma-catalyzed CO₂ hydrogenation to DME[J]. Acta Phys. -Chim. Sin. 2025, 41(6), 100054. doi: 10.1016/j.actphy.2025.100054

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Catalysts	BET surface area (m²∙g⁻¹)	Average pore size (nm)	Pore volume (cm³∙g⁻¹)
Cu/Al₂O₃-0.75	274.52	3.92	0.40
Reduced Cu/Al₂O₃-0	166.42	5.07	0.29
Reduced Cu/Al₂O₃-0.5	213.99	4.57	0.34
Reduced Cu/Al₂O₃-0.75	219.24	4.10	0.32
Reduced Cu/Al₂O₃-1	223.87	5.33	0.42

Catalysts	H₂ Consumption (μmol∙g⁻¹)	Acid amount (μmol∙g⁻¹)
Al₂O₃-0.75	0	253.62
Cu/Al₂O₃-0	185.66	296.62
Cu/Al₂O₃-0.5	163.66	367.60
Cu/Al₂O₃-0.75	176.70	372.67
Cu/Al₂O₃-1	172.93	377.97

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Soft template-induced deep pore structure of Cu/Al₂O₃ for promoting plasma-catalyzed CO₂ hydrogenation to DME

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Soft template-induced deep pore structure of Cu/Al₂O₃ for promoting plasma-catalyzed CO₂ hydrogenation to DME