Zr(OH)4/Fe3O4催化糠醛转移加氢制糠醇的氧空位和羟基协同作用

IF 13.2 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2025-05-16 DOI:10.1016/j.cej.2025.163844

Yue Wang, Xiangyan He, Qi Zhang, Ling Luo, Tianping Lv, Xiuwu Wang, Junhua Zhang

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引用次数: 0

摘要

高效催化剂的构建对于生物基羰基催化转移加氢（CTH）到有价值的化学品和燃料至关重要。在十二烷基苯磺酸钠（SDBS）的调控下，我们成功合成了一系列均匀分散的Zr(OH)4-Fe3O4纳米颗粒，该纳米颗粒对糠醛（FAL）的CTH转化为糠醛醇（FOL）表现出优异的活性。系统表征表明，SDBS有效地修饰了Fe3O4与Zr(OH)4之间的相互作用，从而通过促进缺电子锆位点的构建提高了Lewis酸度。同时，Zr(OH)4-Fe3O4-SDBS中氧空位和表面羟基的存在有利于底物和供氢体的吸附和活化。由于这些协同效应，实现了FAL对FOL的完全转换，具有令人印象深刻的选择性，其翻转频率值高达42.5 h−1。令人鼓舞的是，Zr(OH)4-Fe3O4-SDBS在羰基化合物的CTH中也显示出其普遍性，在重复使用11次循环后，其分离能力显著，且活性和结构保持不变。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Synergy of oxygen vacancies and hydroxyl group for catalytic transfer hydrogenation of furfural to furfuryl alcohol on Zr(OH)4/Fe3O4

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Synergy of oxygen vacancies and hydroxyl group for catalytic transfer hydrogenation of furfural to furfuryl alcohol on Zr(OH)4/Fe3O4

Construction of highly efficient catalysts is crucial for the catalytic transfer hydrogenation (CTH) of bio-based carbonyls to valuable chemicals and fuels. Herein, we successfully synthesized a series of uniformly dispersed Zr(OH)₄-Fe₃O₄ nanoparticles with the regulation of sodium dodecyl benzene sulfonate (SDBS), which exhibited exceptional activity for the CTH of furfural (FAL) into furfuryl alcohol (FOL). Systematic characterizations revealed that SDBS effectively modified the interaction between Fe₃O₄ and Zr(OH)₄, thereby enhancing Lewis acidity by facilitating the construction of electron-deficient zirconium sites. Meanwhile, the presence of oxygen vacancies and surface hydroxyl groups in Zr(OH)₄-Fe₃O₄-SDBS facilitated the adsorption and activation of both substrate and hydrogen donor. Thanks to these synergistic effects, a complete conversion of FAL with an impressive selectivity towards FOL was achieved, with a remarkable turn-over frequency value reaching as high as 42.5 h⁻¹. Encouragingly, Zr(OH)₄-Fe₃O₄-SDBS also demonstrated its universality in the CTH of carbonyl compounds by exhibiting remarkable separation capability while maintaining its activity and structure after being reused for 11 cycles without significant changes.

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来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.