Selective adsorption and hydrogenolysis of C-OH bond in biomass derived furanic compounds over Ni-TT-Nb2O5

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2024-11-12 DOI:10.1016/j.jcat.2024.115844

Zhendong Yu, Zihao Qin, Hongyuan Liu, Shaoyu Yuan, Renjie Huang, Binglin Chen, Zheng Li, Lu Lin, Carol Sze Ki Lin, Xianhai Zeng

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Abstract

The selective hydrogenolysis of C-OH in renewable furanic compounds to corresponding high-value products has been attractive yet challenging, and the mechanism remains vague. Herein, a non-noble catalyst (Ni-TT-Nb₂O₅) was prepared to address this challenge. Batch and continuous reaction results show that Ni-TT-Nb₂O₅ can selectively hydrodeoxygenate 5-hdyroxymethylfurfural to 5-methylfurfural with a very high selectivity of 99 %. Moreover, Ni-TT-Nb₂O₅ can also selectively hydrodeoxygenate various furanic, benzenoid and aliphatic alcohols, achieving up to > 95 % selectivity. In-situ FTIR and DFT calculations showed that compared with other Ni-supported (supports = Al₂O₃, CeO₂, SiO₂, ZrO₂) catalysts, HMF was adsorbed on Ni-TT-Nb₂O₅ surface via parallel mode exclusively, and the C-OH bond was easier to be activated. This work therefore explained the mechanism of selective hydrogenolysis of C-OH in HMF over Ni-TT-Nb₂O₅, and offered an advanced approach for the upgrading of C-OH-containing furanic compounds as well as benzenoid and aliphatic alcohols.

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Ni-TT-Nb2O5 对生物质衍生呋喃化合物中 C-OH 键的选择性吸附和氢解作用

将可再生呋喃化合物中的 C-OH 选择性氢解为相应的高价值产品具有吸引力，但这一过程极具挑战性，其机理仍然模糊不清。本文制备了一种非贵金属催化剂（Ni-TT-Nb2O5）来应对这一挑战。批量和连续反应结果表明，Ni-TT-Nb2O5 可选择性地将 5-羟甲基糠醛加氢脱氧为 5-甲基糠醛，选择性高达 99%。此外，Ni-TT-Nb2O5 还能选择性地加氢脱氧各种呋喃类、苯类和脂肪醇，选择性高达 95%。原位傅立叶变换红外光谱和 DFT 计算表明，与其他镍支撑（支撑物 = Al2O3、CeO2、SiO2、ZrO2）催化剂相比，HMF 完全通过平行模式吸附在 Ni-TT-Nb2O5 表面，C-OH 键更容易被活化。因此，该研究解释了 Ni-TT-Nb2O5 上 HMF 中 C-OH 的选择性氢解机理，为含 C-OH 的呋喃化合物以及苯环和脂肪醇的升级提供了一种先进的方法。

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

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.