基于溶剂调节的生物质平台化合物的可切换氢化化学选择性

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-10 DOI:10.1016/j.apcatb.2024.123719
Yuanjing Zhang , Si Wang , Yusen Yang , Lei Wang , Enze Xu , Quandong Hou , Shiquan Zhao , Tianyong Liu , Song Hong , Lirong Zheng , Feng Li , Xin Zhang , Min Wei
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引用次数: 0

摘要

生物质衍生化合物选择性催化转化为燃料和精细化学品是部分替代化石资源的可再生能源途径,其中反应途径和选择性控制是关键问题。在此,我们报告了一种固定在 CoAl 混合金属氧化物催化剂上的全暴露铂簇合物(简称为 Ptn/CoAl-MMOs),该催化剂在糠醛(FAL)的液相加氢反应中表现出突出的催化性能。值得注意的是,通过使用四种不同的溶剂,氢化化学选择性可在四种产物之间切换:在乙醇、二噁烷、异丙醇和正己烷溶剂中分别获得四氢糠醇 (THFA;收率:91.4%)、糠醇 (FA;收率:97.7%)、2-甲基呋喃 (2-MF;收率:92.1%) 和呋喃 (FU;收率:90.8%)。实验研究(原位傅立叶变换红外光谱和 TPSR-质谱)结合理论计算(DFT)发现,溶剂分子通过改变溶剂-催化剂和/或底物-催化剂之间的相互作用,对 FAL 的吸附构型产生了重要影响,最终决定了氢化途径、关键中间产物和最终产物。这项工作展示了在一个催化体系内实现依赖溶剂的产品切换策略,为在液固催化反应中定制加氢选择性以实现生物质升级开辟了潜在的机会。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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A switchable hydrogenation chemoselectivity of biomass platform compounds based on solvent regulation

Selective catalytic conversion of biomass-derived compounds to fuels and fine chemicals serves as a renewable energy pathway for the partial substitution of fossil resources, in which reaction pathway and selectivity control are key issues. Herein, we report a fully exposed Pt clusters immobilized on CoAl mixed metal oxides catalyst (denoted as Ptn/CoAl-MMOs), which exhibits prominent catalytic performance towards liquid phase hydrogenation reaction of furfural (FAL). Noteworthily, the hydrogenation chemoselectivity can be switched among four products via using four different solvents: tetrahydrofurfuryl alcohol (THFA; yield: 91.4%), furfuryl alcohol (FA; yield: 97.7%), 2-methylfuran (2-MF; yield: 92.1%) and furan (FU; yield: 90.8%) are obtained in ethanol, dioxane, isopropanol and n-hexane solvent, respectively. Experimental studies (in situ FT-IR and TPSR-Mass) combined with theoretical calculations (DFT) reveal that solvent molecules exert an essential influence on the adsorption configuration of FAL via changing the solvent-catalyst and/or substrate-catalyst interaction, which ultimately determines the hydrogenation pathway, key intermediate and final product. This work demonstrates a facile solvent-dependent product-switching strategy within one catalytic system, which opens up potential opportunities for tailoring hydrogenation selectivity in liquid-solid catalytic reactions towards biomass upgrading.

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来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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