Liuyun Chen , Wenju Wang , Tairong Lu , Xuan Luo , Xinling Xie , Kelin Huang , Shanli Qin , Tongming Su , Zuzeng Qin , Hongbing Ji
{"title":"Soft template-induced deep pore structure of Cu/Al2O3 for promoting plasma-catalyzed CO2 hydrogenation to DME","authors":"Liuyun Chen , Wenju Wang , Tairong Lu , Xuan Luo , Xinling Xie , Kelin Huang , Shanli Qin , Tongming Su , Zuzeng Qin , Hongbing Ji","doi":"10.1016/j.actphy.2025.100054","DOIUrl":null,"url":null,"abstract":"<div><div>Plasma-activated heterogeneous catalysis is a promising strategy for catalytic CO<sub>2</sub> hydrogenation under mild conditions. In this study, pore structures with deep pore channels were constructed on Al<sub>2</sub>O<sub>3</sub>-<em>x via</em> a soft template method, and Cu/Al<sub>2</sub>O<sub>3</sub>-<em>x</em> was prepared by an impregnation method, with Al<sub>2</sub>O<sub>3</sub>-<em>x</em> serving as the support for plasma-catalyzed CO<sub>2</sub> hydrogenation to dimethyl ether (DME). Cu/Al<sub>2</sub>O<sub>3</sub>-0.75/HZSM-5 demonstrated a high performance and discharge efficiency for plasma-catalyzed CO<sub>2</sub> hydrogenation. The CO<sub>2</sub> conversion and DME yield for plasma-catalyzed CO<sub>2</sub> hydrogenation on Cu/Al<sub>2</sub>O<sub>3</sub>-0.75/HZSM-5 reached 21.98% and 9.83%, respectively, with selectivities for CO, CH<sub>3</sub>OH, and DME on Cu/Al<sub>2</sub>O<sub>3</sub>-0.75/HZSM-5 of 25.39%, 29.89%, and 44.72%, respectively. The deep pore structures on Al<sub>2</sub>O<sub>3</sub>-<em>x</em> 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 CO<sub>2</sub>. Notably, the electric field formed by Cu sites anchored in the deep pore channel structures is conducive to guiding the activated plasma CO<sub>2</sub> intermediates into the difficult-to-access pores for hydrogenation. Hydrogenation of the plasma-activated CO<sub>2</sub> intermediates in the deep pore channels is crucial for improving plasma-catalyzed CO<sub>2</sub> hydrogenation to DME.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 6","pages":"Article 100054"},"PeriodicalIF":10.8000,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"物理化学学报","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1000681825000104","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
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.