SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2023, Vol. 53 ›› Issue (1): 232-242.DOI: 10.1016/j.cjche.2022.03.001

• Full Length Article • 上一篇    下一篇

Fabrication of hydrophobic Pd/Al2O3-phosphoric acid via P-O-Al bond for liquid hydrogenation reaction

Lu Lv1, Min Zhao1, Yanan Liu1,2, Yufei He1,2, Dianqing Li1,2   

  1. 1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
    2. Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China
  • 收稿日期:2021-09-01 修回日期:2022-03-01 出版日期:2023-01-28 发布日期:2023-04-08
  • 通讯作者: Yanan Liu,E-mail:ynliu@mail.buct.edu.cn;Yufei He,E-mail:yfhe@mail.buct.edu.cn
  • 基金资助:
    This work was supported by National Key Research & Development Program of China (2021YFB3801600), Fundamental Research Funds for the Central University (buctrc201921, JD2223, 12060093063) and Innovative Achievement Commercialization Service-Platform of Industrial Catalysis (2019-00900-2-1).

Fabrication of hydrophobic Pd/Al2O3-phosphoric acid via P-O-Al bond for liquid hydrogenation reaction

Lu Lv1, Min Zhao1, Yanan Liu1,2, Yufei He1,2, Dianqing Li1,2   

  1. 1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
    2. Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China
  • Received:2021-09-01 Revised:2022-03-01 Online:2023-01-28 Published:2023-04-08
  • Contact: Yanan Liu,E-mail:ynliu@mail.buct.edu.cn;Yufei He,E-mail:yfhe@mail.buct.edu.cn
  • Supported by:
    This work was supported by National Key Research & Development Program of China (2021YFB3801600), Fundamental Research Funds for the Central University (buctrc201921, JD2223, 12060093063) and Innovative Achievement Commercialization Service-Platform of Industrial Catalysis (2019-00900-2-1).

摘要: Alumina (Al2O3) is widely used in the chemical industry as the catalyst and support due to its high specific surface area, abundant pore size distribution and chemical stability. However, the occurrence of hydration in water environment, result in outstanding decrease in specific surface area and collapse of pore structure. In this work, dodecyl phosphoric acid (PA) is used to modify the surface of Al2O3 to obtain a series of hydrophobic material (Al2O3-PA). Based on XPS and NMR analysis, PA is chemically bonded on Al2O3 to form P-O-Al bond. Furthermore, BET and WCA results display that Al2O3-1PA exhibits excellent the hydrophobicity and hydrothermal stability while maintains the pore structure. Take it as the substrate to support the Pd nanoparticles, the as-prepared Pd/Al2O3-PA shows the superior catalytic performance in the hydrogenation of phenol and anthraquinone relative to Pd/Al2O3, indicating the accessibility of Pd sites after PA modification. Especially, the significantly enhanced stability is also obtained in four cycles for aqueous phenol hydrogenation. This can be ascribed that the PA modification inhibits the aggregation of Pd nanoparticles and the products adhesion in the reaction process. The extension of PA coatings to monolithic catalysts could expand their current capabilities in industrial applications and warrants ongoing investigation.

关键词: Alumina modification, Hydrophobic catalyst, Phenol hydrogenation, Anthraquinone hydrogenation, Accessible Pd sites

Abstract: Alumina (Al2O3) is widely used in the chemical industry as the catalyst and support due to its high specific surface area, abundant pore size distribution and chemical stability. However, the occurrence of hydration in water environment, result in outstanding decrease in specific surface area and collapse of pore structure. In this work, dodecyl phosphoric acid (PA) is used to modify the surface of Al2O3 to obtain a series of hydrophobic material (Al2O3-PA). Based on XPS and NMR analysis, PA is chemically bonded on Al2O3 to form P-O-Al bond. Furthermore, BET and WCA results display that Al2O3-1PA exhibits excellent the hydrophobicity and hydrothermal stability while maintains the pore structure. Take it as the substrate to support the Pd nanoparticles, the as-prepared Pd/Al2O3-PA shows the superior catalytic performance in the hydrogenation of phenol and anthraquinone relative to Pd/Al2O3, indicating the accessibility of Pd sites after PA modification. Especially, the significantly enhanced stability is also obtained in four cycles for aqueous phenol hydrogenation. This can be ascribed that the PA modification inhibits the aggregation of Pd nanoparticles and the products adhesion in the reaction process. The extension of PA coatings to monolithic catalysts could expand their current capabilities in industrial applications and warrants ongoing investigation.

Key words: Alumina modification, Hydrophobic catalyst, Phenol hydrogenation, Anthraquinone hydrogenation, Accessible Pd sites