ZrO2 stablishing CoO facilitates hydrogenolysis of 5-hydroxymethylfurfural to 2,5-dimethylfuran

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-02-01 Epub Date: 2024-12-12 DOI:10.1016/j.mcat.2024.114765
Kaiyun Lu , Mingxiu Cao , Yuxin Du , Hao Huang , Wenjie Xiang , Guangbo Liu , Jifan Li , Chun-Ling Liu , Noritatsu Tsubaki , Wen-Sheng Dong
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Abstract

The synthesis of high value-added 2,5-dimethylfuran (2,5-DMF) from catalytic hydrogenolysis of 5-hydroxymethylfurfural (5-HMF) is one of significant reactions for biomass utilization, but it still confronts big challenges for the development of base metal catalysts with high performance. In this work, we fabricated series of ZrO2 modified Co nanocatalysts derived from layered double hydroxides (LDHs), wherein metastable state CoO species can be stablished via sacrifice of a portion of surface vacancies, for selective synthesis of 2,5-DMF via 5-HMF hydrogenolysis. The optimal catalyst 2ZrO2-Co/Al2O3 shows great catalytic performance and good stability, which gives a high 2,5-DMF yield of up to 97.3 %. The addition of ZrO2 stablishes the metastable state CoO species, which cooperate with suitable oxygen vacancies and enhance the adsorption of 5-HMF and heterolytic dissociation of H2 to generate highly active Hδ− species, consequently achieving excellent catalytic performance for hydrogenolysis of 5-HMF to 2,5-DMF.

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ZrO2建立CoO有利于5-羟甲基糠醛氢解为2,5-二甲基呋喃
5-羟甲基糠醛(5-HMF)催化氢解合成高附加值的2,5-二甲基呋喃(2,5- dmf)是生物质利用的重要反应之一,但高性能贱金属催化剂的开发仍面临较大挑战。在这项工作中,我们制备了一系列由层状双氢氧化物(LDHs)衍生的ZrO2修饰的Co纳米催化剂,其中通过牺牲部分表面空位可以建立亚稳态CoO物种,通过5-HMF氢解选择性合成2,5- dmf。最佳催化剂2ZrO2-Co/Al2O3具有良好的催化性能和良好的稳定性,可使2,5- dmf收率达到97.3%。ZrO2的加入建立了亚稳态的CoO物种,这些物种与合适的氧空位配合,增强了5-HMF的吸附和H2的异解离解生成高活性的Hδ−物种,从而实现了5-HMF氢解制2,5- dmf的优异催化性能。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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