{"title":"用钴合金化方法提高芳香族硝基苯加氢催化剂碳壳中电子的穿透性","authors":"Wei He, Yanni Li, Qiuyuan Xiang, Xiyuan Zhang, Jiaxin Yu, Chaofan Ma, Yongyue Yao, Chunyu Yin, Yi Liu, Yebin Zhou, Xiaonian Li, Chunshan Lu","doi":"10.1016/j.jcat.2025.116150","DOIUrl":null,"url":null,"abstract":"<div><div>Encapsulated catalysts have become a new strategy for catalysis in harsh reaction environments due to their unique structural and functional reorganization properties, and they have been widely applied in fields such as electrocatalysis, photocatalysis, and thermocatalysis. In strategies involving encapsulated catalysts, the optimization of electronic properties on the carbon layer surface to enhance reactivity while maintaining adequate encapsulation poses a challenge due to the trade-off between stability, poison resistance, and acid resistance against the performance of metal nanoparticles. Herein, an alloying strategy for Co-Ni bimetal was proposed, which achieves a delicate balance between catalyst activity and stability. Ni plays a pivotal role in promoting the formation of graphitized carbon and the construction of an effective encapsulation structure, thereby ensuring the stability of the catalyst. Co incorporation and alloying with Ni modulates the electronic state and D-band structure within the metallic core, effectively breaking the electronic cloud segregation barrier imposed by the carbon shell. This modulation notably enhances the efficiency of reactions. For the hydrogenation of <em>p</em>-CNB to <em>p</em>-CAN, Co<sub>2</sub>Ni<sub>8</sub>@C exhibits an extremely low apparent activation energy (53.40 KJ/mol), as well as > 99 % conversion and selectivity.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116150"},"PeriodicalIF":6.5000,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing electron penetration through carbon shell of encapsulated catalysts by Co alloying for aromatic nitrobenzene hydrogenation\",\"authors\":\"Wei He, Yanni Li, Qiuyuan Xiang, Xiyuan Zhang, Jiaxin Yu, Chaofan Ma, Yongyue Yao, Chunyu Yin, Yi Liu, Yebin Zhou, Xiaonian Li, Chunshan Lu\",\"doi\":\"10.1016/j.jcat.2025.116150\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Encapsulated catalysts have become a new strategy for catalysis in harsh reaction environments due to their unique structural and functional reorganization properties, and they have been widely applied in fields such as electrocatalysis, photocatalysis, and thermocatalysis. In strategies involving encapsulated catalysts, the optimization of electronic properties on the carbon layer surface to enhance reactivity while maintaining adequate encapsulation poses a challenge due to the trade-off between stability, poison resistance, and acid resistance against the performance of metal nanoparticles. Herein, an alloying strategy for Co-Ni bimetal was proposed, which achieves a delicate balance between catalyst activity and stability. Ni plays a pivotal role in promoting the formation of graphitized carbon and the construction of an effective encapsulation structure, thereby ensuring the stability of the catalyst. Co incorporation and alloying with Ni modulates the electronic state and D-band structure within the metallic core, effectively breaking the electronic cloud segregation barrier imposed by the carbon shell. This modulation notably enhances the efficiency of reactions. For the hydrogenation of <em>p</em>-CNB to <em>p</em>-CAN, Co<sub>2</sub>Ni<sub>8</sub>@C exhibits an extremely low apparent activation energy (53.40 KJ/mol), as well as > 99 % conversion and selectivity.</div></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"447 \",\"pages\":\"Article 116150\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2025-04-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021951725002155\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021951725002155","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Enhancing electron penetration through carbon shell of encapsulated catalysts by Co alloying for aromatic nitrobenzene hydrogenation
Encapsulated catalysts have become a new strategy for catalysis in harsh reaction environments due to their unique structural and functional reorganization properties, and they have been widely applied in fields such as electrocatalysis, photocatalysis, and thermocatalysis. In strategies involving encapsulated catalysts, the optimization of electronic properties on the carbon layer surface to enhance reactivity while maintaining adequate encapsulation poses a challenge due to the trade-off between stability, poison resistance, and acid resistance against the performance of metal nanoparticles. Herein, an alloying strategy for Co-Ni bimetal was proposed, which achieves a delicate balance between catalyst activity and stability. Ni plays a pivotal role in promoting the formation of graphitized carbon and the construction of an effective encapsulation structure, thereby ensuring the stability of the catalyst. Co incorporation and alloying with Ni modulates the electronic state and D-band structure within the metallic core, effectively breaking the electronic cloud segregation barrier imposed by the carbon shell. This modulation notably enhances the efficiency of reactions. For the hydrogenation of p-CNB to p-CAN, Co2Ni8@C exhibits an extremely low apparent activation energy (53.40 KJ/mol), as well as > 99 % conversion and selectivity.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.