SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2024, Vol. 72 ›› Issue (8): 60-68.DOI: 10.1016/j.cjche.2024.05.006

• • 上一篇    下一篇

Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

Xin Li, Yue Ma, Xuning Wang, Jianguo Wu, Dong Cao, Daojian Cheng   

  1. State Key Laboratory of Organic-Inorganic Composites and College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • 收稿日期:2023-11-04 修回日期:2024-05-11 出版日期:2024-08-28 发布日期:2024-10-17
  • 通讯作者: Dong Cao,E-mail:caod@mail.buct.edu.cn;Daojian Cheng,E-mail:chengdj@mail.buct.edu.cn
  • 基金资助:
    This work is supported by the National Key Research and Development Program of China (2021YFA1500500).

Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

Xin Li, Yue Ma, Xuning Wang, Jianguo Wu, Dong Cao, Daojian Cheng   

  1. State Key Laboratory of Organic-Inorganic Composites and College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • Received:2023-11-04 Revised:2024-05-11 Online:2024-08-28 Published:2024-10-17
  • Contact: Dong Cao,E-mail:caod@mail.buct.edu.cn;Daojian Cheng,E-mail:chengdj@mail.buct.edu.cn
  • Supported by:
    This work is supported by the National Key Research and Development Program of China (2021YFA1500500).

摘要: The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd0/Pd2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g-C3N4-300 catalyst with a Pd0/Pd2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd0 and Pd2+ in Pd/g-C3N4-300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

关键词: Pd/g-C3N4, Selective hydrogenation, 5-hydroxymethylfurfural, 2,5-dihydroxymethylfuran, Oxidation state

Abstract: The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd0/Pd2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g-C3N4-300 catalyst with a Pd0/Pd2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd0 and Pd2+ in Pd/g-C3N4-300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

Key words: Pd/g-C3N4, Selective hydrogenation, 5-hydroxymethylfurfural, 2,5-dihydroxymethylfuran, Oxidation state