Catalytic oxidation of butylated hydroxytoluene using thermally treated cobalt-copper layered double hydroxides: Synthesis, structural evolution, and mechanistic insights

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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Abstract

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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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

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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来源期刊

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