Cyclohexanone serves as a vital chemical intermediate in nylon production and as a solvent in the manufacturing of resins and paints. The quest for facile, environmentally-friendly, and cost-effective methods to achieve selective oxidation of cyclohexanol is highly desirable. In this study, we successfully achieved the oxidation in water solution using peroxydisulfate (PDS) activation. This was accomplished by employing a Co/N doped porous carbon catalyst synthesized through the one-step carbonization of zeolite-imidazolate frameworks (ZIFs). The catalysts derived from ZIFs with various Co/Zn ratios were extensively characterized using XRD, SEM, TEM, N adsorption–desorption, and XPS techniques. The catalyst's performance was assessed under different reaction conditions, including reaction temperature, PDS dosage, and water quality. Notably, the results revealed that under mild conditions, a high efficiency was achieved with over 55% cyclohexanol conversion and 80% cyclohexanone selectivity within 3 h. To gain a greater understanding of the reactive oxygen species involved, we conducted further quenching experiments and EPR analysis. Our findings suggested that·SO, ·OH, and mediated electron transfer played a dominant role in the oxidation process. The insights obtained from this work have the potential to offer a green and economically viable method for the selective oxidation of cyclohexanol to cyclohexanone.

中文翻译：

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Co/N 掺杂多孔碳上过二硫酸盐选择性氧化环己醇生成环己酮

环己酮是尼龙生产中重要的化学中间体，也是树脂和油漆制造中的溶剂。迫切需要寻找简便、环保且经济有效的方法来实现环己醇的选择性氧化。在这项研究中，我们利用过二硫酸盐（PDS）活化成功实现了水溶液中的氧化。这是通过使用通过沸石-咪唑酯骨架（ZIF）的一步碳化合成的Co/N掺杂多孔碳催化剂来实现的。使用 XRD、SEM、TEM、N 吸附-解吸和 XPS 技术对具有不同 Co/Zn 比例的 ZIF 衍生的催化剂进行了广泛的表征。在不同反应条件下评估催化剂的性能，包括反应温度、PDS用量和水质。值得注意的是，结果表明，在温和条件下，3 小时内实现了高效率，环己醇转化率超过 55%，环己酮选择性达到 80%。为了更好地了解所涉及的活性氧，我们进行了进一步的猝灭实验和 EPR 分析。我们的研究结果表明·SO、·OH 和介导的电子转移在氧化过程中起主导作用。从这项工作中获得的见解有可能为环己醇选择性氧化为环己酮提供一种绿色且经济可行的方法。