Tailored Co/SBA-15 catalyst for highly efficient hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-01-25 DOI:10.1016/j.apcata.2025.120134
Ting Wu, Xiang Zhang, Hongju Liang, Quan Wang, Chun-Ling Liu, Wen-Sheng Dong
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Abstract

The design of highly efficient and cost-effective catalysts for the conversion of biomass-derived 5-hydroxymethylfurfural (5-HMF) into sustainable liquid fuel 2,5-dimethylfuran (DMF) is both important and challenging. In this study, we developed a non-noble Co catalyst supported on SBA-15 (25Co/SBA-15). Our results demonstrate that this catalyst exhibits remarkable efficiency in selectively hydrodeoxygenating 5-HMF to DMF, achieving a DMF yield of 96.3 % with complete conversion of 5-HMF under mild reaction conditions (150 °C, 2.0 MPa H2 for 2 h). Notably, the productivity rate of DMF reached an exceptional value of 19.1 mmol·gcat−1·h−1, surpassing most previously reported catalysts in literature. Additionally, by utilizing two distinct solvents - N,N-dimethylformamide (N,N-DMF) resulting in a high yield of 2,5-bis(hydroxymethyl)furan (BHMF) and tetrahydrofuran (THF) yielding an even higher yield of DMF - our approach enables facile switching between these two products during hydrogenation over the Co/SBA-15 catalyst. Furthermore, our catalyst demonstrates excellent reusability and can be easily regenerated through calcination in air. The exceptional catalytic performance of the catalyst can be ascribed to the synergistic effect between metallic Co and adjacent Lewis acidic Co2+ in CoO dispersed on the surface of SBA-15. A dual-site Langmuir–Hinshelwood–Hougen–Watson (LHHW) model was proposed for the hydrodeoxygenating 5-HMF to DMF.
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定制的Co/SBA-15催化剂用于5-羟甲基糠醛高效加氢脱氧为2,5-二甲基呋喃
设计高效、经济的催化剂将生物质衍生的5-羟甲基糠醛(5-HMF)转化为可持续的液体燃料2,5-二甲基呋喃(DMF)既重要又具有挑战性。在这项研究中,我们开发了一种负载在SBA-15上的非贵金属Co催化剂(25Co/SBA-15)。我们的研究结果表明,该催化剂在选择性加氢脱氧5-HMF到DMF方面表现出显著的效率,在温和的反应条件下(150°C, 2.0 MPa H2, 2 h), 5-HMF完全转化,DMF收率为96.3% %。值得注意的是,DMF的产率达到了19.1 mmol·gcat−1·h−1,超过了文献中报道的大多数催化剂。此外,通过使用两种不同的溶剂- N,N-二甲基甲酰胺(N,N-DMF)产生高产量的2,5-双(羟甲基)呋喃(BHMF)和四氢呋喃(THF)产生更高产量的DMF -我们的方法可以在Co/SBA-15催化剂加氢过程中方便地在这两种产物之间切换。此外,我们的催化剂具有良好的可重复使用性,可以很容易地通过在空气中煅烧再生。催化剂优异的催化性能可归因于分散在SBA-15表面的CoO中金属Co与邻近的Lewis酸性Co2+之间的协同作用。提出了5-羟甲基糠醛加氢脱氧成DMF的双位点Langmuir-Hinshelwood-Hougen-Watson (LHHW)模型。
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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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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