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–N_x 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.

中文翻译：

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通过氮掺杂碳负载的铁原子催化剂的超高分散性增强苯甲醇氧化活性


目前在温和条件下，用高苯甲醇转化率和高苯甲醛选择性难以同时实现苯甲醛的选择性氧化为苯甲醛。在此，通过热分解铁掺杂沸石咪唑骨架前驱体 （x-Fe-ZIF） 制备了锚定在氮掺杂碳 （x-Fe/NC） 上的 Fe 基催化剂。在不同铁含量的多种催化剂 （x-Fe/NC） 中，2-Fe/NC 催化剂表现出最佳的转化率和选择性平衡，苯甲醇转化率达到 96.0%，对苯甲醛的选择性约为 98.0%。一系列表征方法与动力学分析相结合表明，高催化活性归因于形成的 Fe-N_x 活性位点，这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 催化剂表现出优异的可回收性和耐底物性，表明其稳定性和工业应用潜力。本研究为合成有效的过渡金属基催化剂提供了新的视角，并探讨了它们在有机氧化反应中的潜在应用。