物理化学学报 >> 2025, Vol. 41 >> Issue (6): 100054.doi: 10.1016/j.actphy.2025.100054

论文 上一篇    下一篇

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

陈柳云1, 王文举1, 陆泰榕3, 罗轩1, 谢新玲1, 黄科林3, 覃善丽3, 苏通明1,*(), 秦祖赠1,*(), 纪红兵1,2   

  1. 1 广西大学化学化工学院, 南宁 530004
    2 浙江工业大学浙江绿色石化与轻烃转化研究院, 杭州 310014
    3 广西产研院新型功能材料研究所, 南宁 530201
  • 收稿日期:2024-12-22 修回日期:2025-01-21 录用日期:2025-01-21 发布日期:2025-04-19
  • 通讯作者: Email: sutm@gxu.edu.cn (苏通明)qinzuzeng@gxu.edu.cn (秦祖赠)
  • 基金资助:
    国家自然科学基金(22078074); 国家自然科学基金(22208065); 广西科技重大专项(Guike AA24263003)

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

Liuyun Chen1, Wenju Wang1, Tairong Lu3, Xuan Luo1, Xinling Xie1, Kelin Huang3, Shanli Qin3, Tongming Su1,*(), Zuzeng Qin1,*(), Hongbing Ji1,2   

  1. 1 School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China
    2 Zhejiang Green Petrochemical and Light Hydrocarbon Transformation Research Institute, Zhejiang University of Technology, Hangzhou 310014, China
    3 Institute of New Functional Materials of Guangxi Institute of Industrial Technology, Nanning 530201, China
  • Received:2024-12-22 Revised:2025-01-21 Accepted:2025-01-21 Published:2025-04-19
  • Contact: Email: sutm@gxu.edu.cn (Tongming Su)qinzuzeng@gxu.edu.cn (Zuzeng Qin)
  • Supported by:
    the National Natural Science Foundation of China(22078074); the National Natural Science Foundation of China(22208065); the Key Projects of Guangxi Science and Technology(Guike AA24263003)

RichHTML

22

PDF

685

赞

补充材料

1

摘要：

等离子体活化非均相催化反应是在温和条件下实现CO2加氢反应的前沿策略。在本研究中，采用软模板法在Al2O3-x上构建了深孔通道结构。以Al2O3-x作为载体，通过浸渍法制备了Cu/Al2O3-x催化剂，并将其应用于等离子体催化CO2加氢制二甲醚(DME)反应。在等离子体催化CO2加氢反应中，Cu/Al2O3-0.75/HZSM-5展现出高性能和高放电效率。其等离子体催化CO2加氢的CO2转化率和DME产率分别达21.98%和9.83%，其中CO、CH3OH和DME的选择性分别为25.39%、29.89%和44.72%。Al2O3-x上的深孔道结构能够作为Cu的负载位点，同时介孔结构的限域效应增强了金属-载体之间的相互作用及Cu的金属分散度。更丰富且更强的Brønsted碱性和Lewis酸性位点促进了CO2的吸附、活化及加氢。值得注意地，锚定在深孔道结构中的Cu位点能够形成电场，从而引导等离子体活化CO2中间体进入难以接近的孔隙中进行加氢反应。深孔通道中等离子体活化CO2中间体的加氢对于提升等离子体催化CO2加氢制DME反应效率具有重要意义。

关键词: 等离子体催化, CO2加氢, 二甲醚, Al2O3, 孔道

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