Effect of the reorganization of acid sites induced by metal species on TiO2 supports on the conversion of furfural to acetals and ethers

IF 5.2 2区化学 Q1 CHEMISTRY, APPLIED

Catalysis Today Pub Date : 2024-07-08 DOI:10.1016/j.cattod.2024.114936

Qi Fang , Hong Du , Xiumei Liu , Yunjie Ding

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引用次数: 0

Abstract

For the catalytic hydrogenation of furfural (FFR) over supported metal catalysts, acetals and ethers were often observed as by-products when alcohols were used as solvents. The presence of specific acid sites on the catalyst led to the conversion of FFR to acetals and ethers. To understand the effect of the interaction between metal species and oxide supports on the acid properties of catalysts and the conversion of FFR to acetals and ethers, anatase TiO₂ (TiO₂-A), rutile TiO₂ (TiO₂-R) and these TiO₂ supported Ni catalysts were studied as models. The relationship between the acid properties of these samples and FFR conversion pathways in isopropanol was revealed. The interaction between Ni species and TiO₂ supports was found to selectively remove Brønsted acid sites on the TiO₂ supports in the absence of H₂, thereby inhibiting the conversion of FFR to acetals and ethers in N₂. However, the presence of high-pressure H₂ during the reaction induced the formation of new Brønsted acid sites on Ni/TiO₂ catalysts via hydrogen spillover, promoting the acetalization of FFR to acetals and the hydrogenolysis of acetals to ethers. The Ni/TiO₂-A catalyst exhibited higher activity in catalyzing the conversion of FFR to acetals and ethers compared to the Ni/TiO₂-R catalyst. This work provides reference information for the selective regulation of acid-catalyzed reaction pathways of FFR in alcohols.

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金属物种在二氧化钛载体上引起的酸性位点重组对糠醛转化为乙醛和乙醚的影响

在支撑金属催化剂上催化氢化糠醛（FFR）时，当使用醇类作为溶剂时，经常会观察到副产物乙醛和醚。催化剂上特定酸位点的存在导致糠醛转化为乙醛和醚。为了了解金属物种与氧化物载体之间的相互作用对催化剂酸性以及将 FFR 转化为乙缩醛和醚的影响，我们以锐钛矿二氧化钛（TiO2-A）、金红石型二氧化钛（TiO2-R）和这些二氧化钛载体 Ni 催化剂为模型进行了研究。研究揭示了这些样品的酸特性与异丙醇中 FFR 转化途径之间的关系。研究发现，在没有 H2 的情况下，Ni 物种与 TiO2 载体之间的相互作用会选择性地移除 TiO2 载体上的布氏酸位点，从而抑制 FFR 在 N2 中向乙醛和醚的转化。然而，反应过程中高压 H2 的存在会通过氢溢出诱导 Ni/TiO2 催化剂上新的布氏酸位点的形成，从而促进 FFR 向乙醛的缩醛化以及乙醛向醚的氢解。与 Ni/TiO2-R 催化剂相比，Ni/TiO2-A 催化剂在催化 FFR 转化为乙醛和醚时表现出更高的活性。这项工作为选择性调节 FFR 在醇中的酸催化反应途径提供了参考信息。

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

Catalysis Today 化学-工程：化工

CiteScore

11.50

自引率

3.80%

发文量

573

审稿时长

2.9 months

期刊介绍： Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.

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