Yulin Li, Wenjie Du, Jian Wang, Zhuyin Sui and Xiufeng Xu
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引用次数: 0
摘要
ZIF 衍生碳框架为合理设计和构建高性能非贵金属催化剂提供了丰富的平台。本研究通过在 ZIF-8 中用 Co 替代 Zn,然后进行热解,合成了共配位 ZIF 衍生碳框架。由碳纳米管(CNT)包裹的 Co-Zn@C-N 在苯甲醇(BnOH)的选择性氧化过程中表现出卓越的催化性能,室温下的最佳 BnOH 转化率达到 92%,苯甲醛(BzH)选择性达到 92%。表征结果证实,反应是通过自由基机制进行的,Co 纳米粒子催化石墨化形成的 CNT 提供了固液反应界面,并增强了自由基和骨架之间的电子转移。作为主要活性位点的 Co 和 Zn 物种表现出协同效应,使 Co-Zn@N-C 催化剂具有良好的性能。此外,石墨化程度的提高、大量的 Co0 和石墨化 N 共同促进了催化性能的提高。此外,该催化剂还具有极佳的可重复使用性和稳定性,在连续四个实验周期中的活性变化可以忽略不计。这种 Co-Zn@N-C 催化剂体系为设计用于温和条件下有机物氧化反应的高活性非贵金属催化剂奠定了良好的基础。
Co, Zn-coordinated ZIF-derived bimetal encapsulated N-doped CNTs for highly effective oxidation of benzyl alcohol at room temperature†
A ZIF-derived carbon framework offered abundant platforms for the rational design and construction of high-performance nonprecious-metal catalysts. In this study, a Co-coordinated ZIF-derived carbon framework was synthesized by substituting Co for Zn in ZIF-8, followed by pyrolysis. The resultant Co–Zn@C–N, wrapped by carbon nanotubes (CNTs), exhibited superior catalytic performance in the selective oxidation of benzyl alcohol (BnOH), achieving an optimal BnOH conversion of 92% and a benzaldehyde (BzH) selectivity of 92% at room temperature. Characterization results confirmed that the reaction proceeded through a free-radical mechanism, and the CNTs, formed through catalytic graphitization induced by Co nanoparticles, provided solid–liquid reaction interfaces and enhanced the electron transfer between radicals and skeletons. The Co and Zn species, acting as the primary active sites, exhibited a synergistic effect that enabled the good performance of the Co–Zn@N–C catalyst. Moreover, the elevated graphitic degree, substantial content of Co0 and graphitic N collectively contributed to the enhanced catalytic performance. Additionally, the catalyst had excellent reusability and stability, manifesting negligible variations in activity across four consecutive experimental cycles. This Co–Zn@N–C catalyst system provides a promising foundation towards the design of highly active non-noble catalysts for organics oxidation reactions under mild conditions.