使用热处理钴铜层状双氢氧化物催化丁基羟基甲苯氧化:合成、结构演变和机理认识

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-09-21 DOI:10.1016/j.mcat.2024.114484
JiYu Wang, Naiwang Liu, Li Shi, Xuan Meng
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引用次数: 0

摘要

本研究调查了钴铜层状双氢氧化物(LDHs)在丁基羟基甲苯(BHT)氧化中的应用,并探讨了它们在热处理过程中的催化行为。LDHs 是通过共沉淀法合成的,不同比例的 Co-Cu 水滑石均经过热处理。结构分析表明,热处理将 LDHs 转变为混合金属氧化物。在合成的催化剂中,Co1Cu3-LDHs 在 BHT 的氧化过程中表现出更高的催化活性。研究采用了 XRD、FT-IR、TGA、N2 吸附-解吸、SEM 和 XPS 等技术来研究 LDHs 的结构变化和表面性质。在 250 °C 下处理的 Co1Cu3-LDH 催化剂表现出优异的催化性能,这归功于 Co 和 Cu 的协同效应。优化反应条件后,BHT 的转化率达到 99%,对 3,5-二叔丁基-4-羟基苯甲醛(BHT-CHO)的选择性为 77%。氧化机理包括苯环上 π 电子系统的氧化和酚羟甲基的深度氧化,并提出了两种潜在的反应途径。
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Catalytic oxidation of butylated hydroxytoluene using thermally treated cobalt-copper layered double hydroxides: Synthesis, structural evolution, and mechanistic insights

This study investigates the application of cobalt-copper layered double hydroxides (LDHs) in the oxidation of butylated hydroxytoluene (BHT) and explores their catalytic behavior during thermal treatment. LDHs were synthesized via coprecipitation, and various ratios of Co-Cu hydrotalcite were subjected to thermal treatment. Structural analysis revealed that thermal treatment transforms the LDHs into mixed metal oxides. Among the synthesized catalysts, Co1Cu3-LDHs exhibited superior catalytic activity in the oxidation of BHT. Techniques such as XRD, FT-IR, TGA, N2 adsorption-desorption, SEM, and XPS were employed to investigate the structural changes and surface properties of the LDHs. The Co1Cu3-LDH catalyst, treated at 250 °C, exhibited outstanding catalytic performance, attributed to the synergistic effects between Co and Cu. Upon optimizing the reaction conditions, the conversion of BHT reached 99 %, with a selectivity of 77 % towards 3,5-di‑tert‑butyl‑4-hydroxybenzaldehyde (BHT-CHO). The oxidation mechanism involves the oxidation of the π-electron system on the benzene ring and deep oxidation of the phenolic hydroxyl methyl group, with two potential reaction pathways proposed.

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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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