{"title":"层状硅酸盐镍衍生金属酸双官能团Ni/SiO2催化剂用于醇的选择性还原胺化反应","authors":"Qiongjin Jiang, Shiyi Rao, Zhenyu Yang, Xiao Fu, Weikun Chen, Linmin Ye , Youzhu Yuan","doi":"10.1016/j.apcata.2025.120310","DOIUrl":null,"url":null,"abstract":"<div><div>The reductive amination of alcohols offers a cost-effective and sustainable pathway for the synthesis of amines. However, achieving high selectivity for primary amines remains a challenge. Herein, we report a nickel phyllosilicate catalyst (Ni/SiO<sub>2</sub>-AE) synthesized via ammonia evaporation, which demonstrates superior catalytic performance with 53.2% alcohol conversion and 96.2% primary amine selectivity. This outperforms conventional Ni/SiO<sub>2</sub> catalysts prepared by impregnation (16.5% conversion, 98.6% selectivity) and deposition-precipitation (41.3% conversion, 94.5% selectivity). The Ni/SiO<sub>2</sub>-AE catalyst exhibits remarkable stability over five reaction cycles, demonstrating both durability and recyclability. Characterization studies reveal that the high catalytic performance stems from the synergy between highly dispersed Ni<sup>0</sup> nanoparticles and Lewis acid sites derived from unsaturated Ni(II) species, which facilitate alcohol adsorption and activation. Additionally, the robust skeletal structure of nickel phyllosilicate contributes to the recyclability of the Ni/SiO<sub>2</sub>-AE catalyst. The metal–acid bifunctional Ni/SiO<sub>2</sub>-AE catalyst also displays broad substrate applicability, effectively converting diverse alcohols into their corresponding primary amines.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120310"},"PeriodicalIF":4.7000,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Nickel phyllosilicate derived metal–acid bifunctional Ni/SiO2 catalysts for selective reductive amination of alcohols\",\"authors\":\"Qiongjin Jiang, Shiyi Rao, Zhenyu Yang, Xiao Fu, Weikun Chen, Linmin Ye , Youzhu Yuan\",\"doi\":\"10.1016/j.apcata.2025.120310\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The reductive amination of alcohols offers a cost-effective and sustainable pathway for the synthesis of amines. However, achieving high selectivity for primary amines remains a challenge. Herein, we report a nickel phyllosilicate catalyst (Ni/SiO<sub>2</sub>-AE) synthesized via ammonia evaporation, which demonstrates superior catalytic performance with 53.2% alcohol conversion and 96.2% primary amine selectivity. This outperforms conventional Ni/SiO<sub>2</sub> catalysts prepared by impregnation (16.5% conversion, 98.6% selectivity) and deposition-precipitation (41.3% conversion, 94.5% selectivity). The Ni/SiO<sub>2</sub>-AE catalyst exhibits remarkable stability over five reaction cycles, demonstrating both durability and recyclability. Characterization studies reveal that the high catalytic performance stems from the synergy between highly dispersed Ni<sup>0</sup> nanoparticles and Lewis acid sites derived from unsaturated Ni(II) species, which facilitate alcohol adsorption and activation. Additionally, the robust skeletal structure of nickel phyllosilicate contributes to the recyclability of the Ni/SiO<sub>2</sub>-AE catalyst. The metal–acid bifunctional Ni/SiO<sub>2</sub>-AE catalyst also displays broad substrate applicability, effectively converting diverse alcohols into their corresponding primary amines.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"701 \",\"pages\":\"Article 120310\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-04-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X2500211X\",\"RegionNum\":2,\"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":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X2500211X","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Nickel phyllosilicate derived metal–acid bifunctional Ni/SiO2 catalysts for selective reductive amination of alcohols
The reductive amination of alcohols offers a cost-effective and sustainable pathway for the synthesis of amines. However, achieving high selectivity for primary amines remains a challenge. Herein, we report a nickel phyllosilicate catalyst (Ni/SiO2-AE) synthesized via ammonia evaporation, which demonstrates superior catalytic performance with 53.2% alcohol conversion and 96.2% primary amine selectivity. This outperforms conventional Ni/SiO2 catalysts prepared by impregnation (16.5% conversion, 98.6% selectivity) and deposition-precipitation (41.3% conversion, 94.5% selectivity). The Ni/SiO2-AE catalyst exhibits remarkable stability over five reaction cycles, demonstrating both durability and recyclability. Characterization studies reveal that the high catalytic performance stems from the synergy between highly dispersed Ni0 nanoparticles and Lewis acid sites derived from unsaturated Ni(II) species, which facilitate alcohol adsorption and activation. Additionally, the robust skeletal structure of nickel phyllosilicate contributes to the recyclability of the Ni/SiO2-AE catalyst. The metal–acid bifunctional Ni/SiO2-AE catalyst also displays broad substrate applicability, effectively converting diverse alcohols into their corresponding primary amines.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.