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Efficient synthesis of the liquid fuel 2,5-dimethylfuran from biomass derived 5-(chloromethyl)furfural at room temperature
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-13 , DOI: 10.1016/j.apcatb.2022.121842
Binglin Chen , Yunchao Feng , Renjie Huang , Shibo Yang , Zheng Li , Jonathan Sperry , Shuliang Yang , Xing Tang , Yong Sun , Lu Lin , Xianhai Zeng

The synthesis of renewable transportation fuel 2,5-dimethylfuran (DMF) from biomass is a promising solution for efficient alleviating the dependence on the petroleum-derived commodities. Here, we found that in-situ generation of acidic species and Pd-Cl active sites bring high selectivity and activity towards hydrogenolysis of biomass-derived 5-(chloromethyl)furfural (CMF) to DMF. Gratifyingly, 92% DMF yield was achieved from CMF for 15 min, which indicates that space-time-yield is at least one order of magnitude higher than previous literature employed 5-hydroxymethylfurfural (HMF) as substrate. Kinetic studies showed that the in-situ formed acid has ignorable negative effect on polymerization of substrate to humins. DFT explicitly elucidate that the decorated Pd nanoparticles by Cl species provided lower adsorption energy and energy of C-O cleavage than Pd sites. Furthermore, the strategy of in-situ formation of homogeneous acid and halogen-modified metal is also efficient for catalytic conversion of other chlorinated carboxides to hydrocarbons with the ring intact.



中文翻译:

室温下从生物质衍生的 5-(氯甲基)糠醛高效合成液体燃料 2,5-二甲基呋喃

从生物质中合成可再生运输燃料 2,5-二甲基呋喃 (DMF) 是有效缓解对石油衍生商品依赖的有前景的解决方案。在这里,我们发现酸性物质和 Pd-Cl 活性位点的原位生成为生物质衍生的 5-(氯甲基)糠醛 (CMF) 氢解为 D​​MF 带来了高选择性和活性。令人欣慰的是,CMF 在 15 分钟内获得了 92% 的 DMF 产率,这表明时空产率比以前使用 5-羟甲基糠醛 (HMF) 作为底物的文献高出至少一个数量级。动力学研究表明,原位生成的酸对底物聚合为腐殖质具有可忽略的负面影响。DFT 明确地阐明了由 Cl 物种修饰的 Pd 纳米粒子提供的吸附能和 CO 裂解能量低于 Pd 位点。此外,原位形成均相酸和卤素改性金属的策略对于将其他氯化碳氧化物催化转化为环完整的烃也是有效的。

更新日期:2022-08-17
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