羧化UiO-66金属-有机骨架负载镍催化剂在温和条件下糠醛加氢制四氢糠醇

IF 6.2 2区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Analytical and Applied Pyrolysis Pub Date : 2026-05-01 Epub Date: 2026-01-14 DOI:10.1016/j.jaap.2026.107616

Shuailong Dong , Bo Cai , Xinyi Luo , Mengyao Chen , Hui Pan

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引用次数: 0

摘要

选择性加氢是将生物质衍生化合物转化为增值化学品的重要途径。本研究制备了羧基化金属-有机骨架UiO-66-(COOH)2，并采用简单浸渍法制备了负载ni催化剂。制备的8Ni/ uuo -66-(COOH)2催化剂在温和条件下（120℃，2 MPa H2, 3 h）可实现糠醛（FAL）的完全转化，四氢糠醇（THFOL）的选择性收率超过97 %。XPS和Py-FTIR表征表明，羧基的引入不仅增加了催化剂的酸性位点，而且促进了UiO-66与金属Ni之间的相互作用，形成富电子的Ni0物质。催化剂中毒试验证实了酸区在FAL加氢过程中的关键作用。认为金属Ni与羧化UiO-66载体的协同作用是8Ni/UiO-66-(COOH)2具有优异催化活性的原因。此外，FAL在8Ni/UiO-66-(COOH)2催化剂上的特异性化学吸附促进了FAL高度选择性加氢成THFOL。根据表征和实验结果，提出了在8Ni/UiO-66-(COOH)2催化剂上催化FAL加氢制THFOL的可能反应途径。

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Carboxylated UiO-66 metal-organic framework-supported nickel catalyst for hydrogenation of furfural to tetrahydrofurfuryl alcohol under mild conditions

Selective hydrogenation is an important pathway to convert biomass-derived compounds to value-added chemicals. In this study, carboxylated metal-organic frameworks UiO-66-(COOH)₂ were prepared and used as a support to fabricate Ni-loaded catalyst by a simple impregnation method. The as-prepared catalyst 8Ni/UiO-66-(COOH)₂ could achieve a complete conversion of furfural (FAL) with a high selective yield of tetrahydrofurfuryl alcohol (THFOL) over 97 % under mild conditions (120 °C, 2 MPa H₂, 3 h). The XPS, Py-FTIR characterization showed that the introduction of a carboxyl group not only increased the acidic site of the catalyst, but also boosted the interaction between UiO-66 and metal Ni to form electron-rich Ni⁰ species. The catalyst poisoning test confirmed the critical role of the acid site in the hydrogenation of FAL. It is believed that the synergistic effect of metallic Ni and the carboxylated UiO-66 support contributed to the excellent catalytic activity of 8Ni/UiO-66-(COOH)₂. Moreover, the specific chemical adsorption of FAL on catalyst 8Ni/UiO-66-(COOH)₂ promoted the highly selective hydrogenation of FAL to THFOL. Based on the characterization and experiment results, a possible reaction pathway of the hydrogenation of FAL to THFOL over catalyst 8Ni/UiO-66-(COOH)₂ is proposed.

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来源期刊

Journal of Analytical and Applied Pyrolysis 化学-分析化学

CiteScore

9.10

自引率

11.70%

发文量

340

审稿时长

44 days

期刊介绍： The Journal of Analytical and Applied Pyrolysis (JAAP) is devoted to the publication of papers dealing with innovative applications of pyrolysis processes, the characterization of products related to pyrolysis reactions, and investigations of reaction mechanism. To be considered by JAAP, a manuscript should present significant progress in these topics. The novelty must be satisfactorily argued in the cover letter. A manuscript with a cover letter to the editor not addressing the novelty is likely to be rejected without review.