物理化学学报 >> 2022, Vol. 38 >> Issue (10): 2204037.doi: 10.3866/PKU.WHXB202204037

所属专题: 生物质催化转化

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Pt/NbPWO双功能催化剂的制备及氢解碱木质素制备芳香单体

曹美芳1, 陈博1, 阮涛1, 欧阳新平1,*(), 邱学青2,*()   

  1. 1 华南理工大学化学与化工学院广东省绿色化学产品技术重点实验室, 广州 510640
    2 广东工业大学轻工化工学院, 广州 510006
  • 收稿日期:2022-04-20 录用日期:2022-05-17 发布日期:2022-05-23
  • 通讯作者: 欧阳新平,邱学青 E-mail:ceouyang@scut.edu.cn;cexqqiu@scut.edu.cn
  • 基金资助:
    国家重点研发项目(2019YFC1905301);国家自然科学基金(22078115);国家自然科学基金(21776108);国家自然科学基金(21690083);国家自然科学基金(22008078)

Preparation of a Pt/NbPWO Bifunctional Catalyst for the Hydrogenolysis of Alkali Lignin to Aromatic Monomers

Meifang Cao1, Bo Chen1, Tao Ruan1, Xinping Ouyang1,*(), Xueqing Qiu2,*()   

  1. 1 School of Chemistry and Chemical Engineering, Guangdong Provincial Key Lab of Green Chemical Product Technology, South China University of Technology, Guangzhou 510640, China
    2 School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China
  • Received:2022-04-20 Accepted:2022-05-17 Published:2022-05-23
  • Contact: Xinping Ouyang,Xueqing Qiu E-mail:ceouyang@scut.edu.cn;cexqqiu@scut.edu.cn
  • About author:Email: cexqqiu@scut.edu.cn (X.Q.)
    Email: ceouyang@scut.edu.cn (X.O.)
  • Supported by:
    the National Key Research and Development Program of China(2019YFC1905301);National Natural Science Foundation of China(22078115);National Natural Science Foundation of China(21776108);National Natural Science Foundation of China(21690083);National Natural Science Foundation of China(22008078)

摘要:

木质素是一种天然芳香族聚合物,约占木质纤维素的30%,是唯一通过裂解C―O醚键和C―C键生产芳香族化学品或液体燃料的可再生芳香族资源。迄今为止,对木质素氢解制备有价值化合物的研究主要集中在相对不稳定的C―O键的裂解上,这限制了木质素氢解的效率。采用水热法和湿浸渍法制备了多功能Pt/NbPWO催化剂。通过破坏碱木质素中的C―O键和C―C键,可以得到产率为18.02%的芳香族单体。该反应不仅可以断裂木质素聚合物中醚键,同时也可以断裂部分关键的C―C键。其氢解机理可能是丰富的Brønsted酸和Lewis酸位点参与了C―C的活化。此外,重点分析载体和Pt物种在Pt/NbPWO催化剂中的协同作用。

关键词: 碱木质素, 双功能催化剂, Brønsted酸和Lewis酸, 协同效应

Abstract:

Lignin is a natural aromatic polymer that accounts for nearly 30% of lignocellulose and is considered the only renewable aromatic (re)source for producing aromatic chemicals or liquid fuels via the cleavage of C―O ether bonds and C―C bonds. Thus far, the majority of investigations involving the production of valuable compounds via lignin hydrogenolysis have focused on the cleavage of relatively labile C―O bonds only, which restricts the efficiency of hydrogenolysis. Therefore, in this work, a bifunctional Pt/NbPWO catalyst was synthesized using hydrothermal and wet impregnation methods. It was found that aromatic monomers with a yield of 18.02% could be obtained by breaking the C―O and C―C bonds in alkali lignin. This reaction was applicable to breaking the key C―C bonds when the C―O ether bonds were broken in lignin polymers. The hydrogenolysis mechanism most likely involves the abundant Brønsted acid and Lewis acid sites on the catalyst that facilitate C―C bond activation. Additionally, the synergy between the support and Pt species in the Pt/NbPWO catalyst was primarily emphasized.

Key words: Alkali lignin, Bifunctional catalyst, Brønsted and Lewis acids, Synergistic effects

MSC2000: 

  • O643