Ceria Nanoparticles on Modified MXene for Aerobic Oxidation of 4-Methoxybenzyl Alcohol

IF 5.3 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Nano Materials Pub Date : 2024-07-10 DOI:10.1021/acsanm.4c02758

Deqiong Xie, Kecan Dou, Jiale Huang, Wenqian Zhai, Jing Shi, Lei Zhuang, Weidong Zhu, Fumin Zhang

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Abstract

The development of efficient and robust metal nanoparticle catalysts for the aerobic oxidation of benzyl alcohol is crucial for advancing green chemistry. This study presents a class of ceria nanoparticle catalysts, designated as Ce-NC/CFMX-T, where “T” denotes the pyrolysis temperature. These catalysts are synthesized by pyrolyzing a mixture of Ce-MOF-801/CFMX and dicyandiamide at high temperatures, aimed at the liquid-phase aerobic oxidation of 4-methoxybenzyl alcohol to 4-methoxybenzaldehyde, using molecular oxygen as the oxidizing agent and avoiding harmful additives or bases. Among the synthesized catalysts, Ce-NC/CFMX-973 exhibited exceptional catalytic efficiency, achieving over 99.9% conversion of 4-methoxybenzyl alcohol and complete selectivity for 4-methoxybenzaldehyde. This performance was achieved under moderate conditions, using xylene as the solvent at 373 K over 8 h and an oxygen pressure of 1 atm. Kinetic analysis revealed that the activation energy for oxidizing 4-methoxybenzyl alcohol using Ce-NC/CFMX-973 was 68.5 ± 3.0 kJ/mol, which is lower than the values observed for Ce-C/CFMX-973, Ce-NC-973, and Ce-C-973. The remarkable catalytic performance of the Ce-NC/CFMX-973 catalyst is attributed to the synergistic effects between CeO₂ nanoparticles and oxygen vacancies, along with the support’s balanced acidity and basicity properties.

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用于 4-甲氧基苄醇有氧氧化的改性 MXene 上的铈纳米粒子

开发用于苯甲醇有氧氧化的高效、坚固的金属纳米粒子催化剂对于推进绿色化学至关重要。本研究提出了一类铈纳米颗粒催化剂，命名为 Ce-NC/CFMX-T，其中 "T "表示热解温度。这些催化剂是通过高温热解 Ce-MOF-801/CFMX 和双氰胺的混合物合成的，目的是利用分子氧作为氧化剂，避免使用有害的添加剂或碱，将 4-甲氧基苯甲醇液相有氧氧化成 4-甲氧基苯甲醛。在合成的催化剂中，Ce-NC/CFMX-973 的催化效率非常高，4-甲氧基苯甲醇的转化率超过 99.9%，对 4-甲氧基苯甲醛具有完全的选择性。这一性能是在中等条件下实现的，以二甲苯为溶剂，在 373 K 和 1 atm 氧气压力下进行了 8 小时的反应。动力学分析表明，使用 Ce-NC/CFMX-973 氧化 4-甲氧基苯甲醇的活化能为 68.5 ± 3.0 kJ/mol，低于在 Ce-C/CFMX-973、Ce-NC-973 和 Ce-C-973 中观察到的值。Ce-NC/CFMX-973 催化剂出色的催化性能归功于 CeO2 纳米粒子和氧空位之间的协同效应，以及载体的酸碱性平衡特性。

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来源期刊

ACS Applied Nano Materials Multiple-

CiteScore

8.30

自引率

3.40%

发文量

1601

期刊介绍： ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.