In-situ generated hydrogen for selective hydrogenolysis of lignin catalyzed by Mg-Al mixed oxides with nested Ni nanoparticles

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-11-02 DOI:10.1016/j.jcat.2024.115833
Yun Tian , Mengqiao Gao , Zhiyang Tang , Fukun Li , Qiang Zeng , Jinxing Long , Xuehui Li
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Abstract

Conversion of lignin to valuable chemicals without external hydrogen presents a significative but challengeable endeavor. Herein, an efficient approach has been proposed for the lignin hydrogenolysis with in-situ hydrogen in the presence of Ni nanoparticles nested in layered double oxides (LDOs). 84.4 % conversion of lignin was achieved over 30Ni-Mg3Al-LDOs, affording a 21.3 % yield of monomers, and 38.0 % of which was identified as 4-ethylphenol. Catalyst characterizations revealed that this excellent performance of lignin conversion should be ascribed to the highly dispersed Ni nanoparticles, strong interfacial interactions between Ni and LDOs, and suitable basicity of catalysts. Furthermore, the roles of the solvent (1,4-dioxane aqueous solution) and the lignin methoxyl groups as hydrogen resources were distinguished, and the former acted as an initial hydrogen to promote lignin depolymerization, and the latter was responsible for the high yield of 4-ethylphenol. In addition, a plausible reaction pathway for lignin hydrogenolysis has been proposed.

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镁铝混合氧化物与嵌套镍纳米颗粒催化木质素选择性氢解产生的原位氢气
在没有外部氢气的情况下将木质素转化为有价值的化学品是一项意义重大但极具挑战性的工作。本文提出了一种在层状双氧化物(LDOs)中嵌套镍纳米粒子的情况下利用原位氢气进行木质素氢解的有效方法。在 30Ni-Mg3Al-LDOs 上,木质素的转化率达到 84.4%,单体产率为 21.3%,其中 38.0%被鉴定为 4-乙基苯酚。催化剂特性分析表明,木质素转化的优异性能应归功于高度分散的镍纳米颗粒、镍与 LDOs 之间强烈的界面相互作用以及催化剂合适的碱性。此外,还区分了溶剂(1,4-二氧六环水溶液)和木质素甲氧基作为氢资源的作用,前者是促进木质素解聚的初始氢,后者是 4-乙基苯酚高产率的原因。此外,还提出了木质素氢解的合理反应途径。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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