氢解
催化作用
丙二醇
甘油
氧气
1,3-丙二醇
空位缺陷
材料科学
化学
化学工程
有机化学
结晶学
工程类
作者
Malin Eqi,Yuqing Yang,Guangjun Wu,Landong Li,Yuchao Chai
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2025-03-12
卷期号:15 (6): 5142-5154
被引量:36
标识
DOI:10.1021/acscatal.5c00547
摘要
The hydrogenolysis of biomass-derived glycerol to 1,3-propanediol is an important process in biomass valorization, while the selective cleavage of the secondary hydroxyl group (C 2 –OH) in glycerol remains a key challenge in chemistry and catalysis. We report herein a multistep approach for the construction of Pt/WO x /Nb 2 O 5 featuring abundant oxygen vacancies and strong Pt δ+ –O–W interactions thereof, making Pt/WOx/Nb 2 O 5 a robust catalyst for glycerol hydrogenolysis to 1,3-propanediol. Typically, the optimized Pt/WO x /Nb 2 O 5 catalyst achieves remarkable performance in the hydrogenolysis of a high-concentration glycerol solution (50.0 wt %) with a glycerol conversion of 94.9%, a 1,3-propanediol selectivity of 67.3%, and a glycerol space-time yield of 0.490 g g cat –1 h –1, surpassing all known catalyst systems. The presence of abundant oxygen vacancies in Pt/WO x /Nb 2 O 5 is directly visualized by microscopy, and the essential role of Pt δ+ –O–W interactions in the reaction is well interpreted by spectroscopic analysis. The Pt δ+ –O–W interactions can promote the selective adsorption of the secondary hydroxyl group in glycerol and the hydrogen spillover from Pt to WO x for in situ Brønsted acid site generation, both facilitating the selective hydrogenolysis of glycerol to 1,3-propanediol. Overall, we show here a successful example of catalyst design via oxygen vacancy engineering for an important process, biomass valorization.
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