Enhanced Activity in Benzyl Alcohol Oxidation via Nitrogen-Doped Carbon-Supported Ultrahigh Dispersion of Iron Atom Catalysts

IF 3.8 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Fan Xue, Shangpu Zhuang, Jingyue Bi, Mifen Cui, Zhaoyang Fei, Xu Qiao
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Abstract

The selective oxidation of benzyl alcohol to benzaldehyde is currently difficult to achieve with high benzyl alcohol conversion and high benzaldehyde selectivity simultaneously under mild conditions. Herein, the Fe-based catalysts anchored on nitrogen-doped carbon (x-Fe/NC) were prepared by thermal decomposition of the iron-doped zeolitic imidazolate framework precursors (x-Fe-ZIF). Among the various catalysts with different iron contents (x-Fe/NC), the 2-Fe/NC catalyst showed the best balance of conversion and selectivity, achieving 96.0% conversion of benzyl alcohol and around 98.0% selectivity for benzaldehyde. A range of characterization methods combined with kinetic analysis demonstrated that the high catalytic activity was attributed to the formed Fe–Nx active sites, which can accelerate the adsorption process of reactant molecules, facilitating the oxidation process while minimizing overoxidation to carboxylic acids. Moreover, the 2-Fe/NC catalyst showed excellent recyclability and substrate resistance, indicating its stability and potential for industrial application. This study offers fresh perspectives on the synthesis of effective transition metal-based catalysts and explores their potential applications in organic oxidation reactions.

Abstract Image

氮掺杂碳负载的超高分散铁原子催化剂增强苯甲醇氧化活性
目前在温和条件下实现高苯甲醇转化率和高苯甲醛选择性同时发生的苯甲醇选择性氧化制苯甲醛的方法比较困难。本文通过对铁掺杂的沸石咪唑酸骨架前驱体(x-Fe- zif)进行热分解制备了锚定在氮掺杂碳上的铁基催化剂(x-Fe/NC)。在不同铁含量(x-Fe/NC)的催化剂中,2-Fe/NC催化剂表现出最佳的转化率和选择性平衡,对苯甲醇的转化率为96.0%,对苯甲醛的选择性为98.0%左右。一系列表征方法结合动力学分析表明,高催化活性归因于形成的Fe-Nx活性位点,它可以加速反应物分子的吸附过程,促进氧化过程,同时最大限度地减少对羧酸的过度氧化。此外,2-Fe/NC催化剂表现出良好的可回收性和耐衬底性,表明其稳定性和工业应用潜力。本研究为高效过渡金属基催化剂的合成提供了新的视角,并探索了其在有机氧化反应中的潜在应用。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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