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

doi:10.1016/j.cjche.2022.03.001

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 Liu^1,2, Yufei He^1,2, Dianqing Li^1,2

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 Liu^1,2, Yufei He^1,2, Dianqing Li^1,2

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/Abstract

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

Lu Lv, Min Zhao, Yanan Liu, Yufei He, Dianqing Li. Fabrication of hydrophobic Pd/Al₂O₃-phosphoric acid via P-O-Al bond for liquid hydrogenation reaction[J]. 中国化学工程学报, 2023, 53(1): 232-242.

Lu Lv, Min Zhao, Yanan Liu, Yufei He, Dianqing Li. Fabrication of hydrophobic Pd/Al₂O₃-phosphoric acid via P-O-Al bond for liquid hydrogenation reaction[J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 232-242.

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

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

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