王东伟,马占伟,李静,冯虎林,胡斌.溶剂诱导法制备不同形貌ZIF-67衍生Co@NC催化剂对苯酚加氢活性的影响[J].分子催化,2024,38(5):399-408 |
溶剂诱导法制备不同形貌ZIF-67衍生Co@NC催化剂对苯酚加氢活性的影响 |
Effect of Different Morphologies Induced by Solvent on ZIF-67 Derived Co@NC for Catalytic Phenol Hydrogenation |
投稿时间:2024-06-11 修订日期:2024-07-15 |
DOI:10.16084/j.issn1001-3555.2024.05.001 |
中文关键词: 金属有机骨架 钴基催化剂 形貌 苯酚加氢 |
英文关键词:metal organic frameworks Co-based catalyst morphology phenol hydrogenation |
基金项目:The National Natural Science Foundation of China (22102194); The Science and Technology Plan of Gansu Province (20JR10RA044); The Youth Innovation Promotion Association of CAS (2022427). |
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中文摘要: |
通过溶剂控制生长和氩气气氛热解两步法制备了不同形貌的Co@NC催化剂, 得到了具有多面体形貌的Co@NC-67P-450和具有叶片状的Co@NC-67L-450. 以苯酚加氢为研究对象评价了两个催化剂的性能, 在160 ℃, 3 MPa的条件下, 环己醇的选择性均在99.9%以上, Co@NC-67P-450催化剂的苯酚转化率为96.9%, 高于Co@NC-67L-450催化剂的75.4%. 在反应过程中, Co3O4被还原为Co0, Co@NC-67P-450的CoNx含量为47.2%, 高于Co@NC-67L-450 (33.4%), 这些共同促进了其苯酚加氢活性. 同时以氨合成为探针反应, 研究了CoNx对N2和H2的催化活性, 进一步证实了其对苯酚加氢活性的促进作用. 通过磁分离可以回收钴基催化剂, 并表现出较高的稳定性. |
英文摘要: |
The Co@NC catalysts with different morphologies were prepared by two step process, solvent control growth and pyrolysis method. The polyhedral Co@NC-67P-450 catalyst has a relatively high CoNx content and exhibits excellent phenol hydrogenation activity (conversion 96.9%) at 160 ℃, 3 MPa, which is higher than that of leaf shaped Co@NC-67L-450 catalyst (conversion 75.4%). We demonstrated Co3O4 was reduced to the Co0 during the reaction. Moreover, CoNx species contribute to the superior hydrogenation activity of phenol. The Co-based catalysts can be easily recovered through the magnetic separation and performed the high stability. |
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