{"title":"mof - 808aa异相催化剂在α-酮酰胺转移加氢反应中的合成及催化应用","authors":"Anuprita A. Mathkar, Bhalchandra M. Bhanage","doi":"10.1016/j.mcat.2025.115167","DOIUrl":null,"url":null,"abstract":"<div><div>In this study, MOF-808 AA was synthesized by modulating the ratio of DMF to acetic acid, and its catalytic performance was evaluated in the transfer hydrogenation of α-keto amides using isopropanol (IPA) as a green hydrogen source and solvent. Furthermore, the methanol activation method was successfully applied to modify MOF-808 AA, resulting in a significantly enhanced catalyst that surpasses the performance of its pristine counterpart in the catalytic transfer hydrogenation (CTH) of α-keto amides. The catalytic conversion of α-keto amide to α‑hydroxy amide proceeded with remarkable efficiency, yielding 84–99 % conversion within a remarkably brief reaction period of 30 min. This protocol showcased remarkable catalytic versatility, efficiently converting a diverse range of α-keto amides, both activating and deactivating substituents on the aniline ring and benzene rings attached to the keto group. A comprehensive characterization of the material's physicochemical properties was conducted using a range of analytical techniques, including, PXRD, nitrogen adsorption-desorption, ammonia TPD, TGA, XPS, FTIR, SEM-EDX, CHN(O) analysis, and ICP-OES. These techniques thoroughly understood the material's structure, composition, and properties. M-MOF 808 AA demonstrated exceptional stability and reusability as a true heterogeneous catalyst, maintaining its activity without any discernible loss over at least four consecutive reaction cycles. A gram-scale conversion was successfully achieved to demonstrate the bulk scalability and industrial potential of the methanol-activated MOF-808 AA catalyst, highlighting its promise for large-scale synthesis and applications.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"582 ","pages":"Article 115167"},"PeriodicalIF":3.9000,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synthesis and catalytic application of MOF-808 AA as heterogeneous catalyst in catalytic transfer hydrogenation reactions of α-Keto amides\",\"authors\":\"Anuprita A. Mathkar, Bhalchandra M. Bhanage\",\"doi\":\"10.1016/j.mcat.2025.115167\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this study, MOF-808 AA was synthesized by modulating the ratio of DMF to acetic acid, and its catalytic performance was evaluated in the transfer hydrogenation of α-keto amides using isopropanol (IPA) as a green hydrogen source and solvent. Furthermore, the methanol activation method was successfully applied to modify MOF-808 AA, resulting in a significantly enhanced catalyst that surpasses the performance of its pristine counterpart in the catalytic transfer hydrogenation (CTH) of α-keto amides. The catalytic conversion of α-keto amide to α‑hydroxy amide proceeded with remarkable efficiency, yielding 84–99 % conversion within a remarkably brief reaction period of 30 min. This protocol showcased remarkable catalytic versatility, efficiently converting a diverse range of α-keto amides, both activating and deactivating substituents on the aniline ring and benzene rings attached to the keto group. A comprehensive characterization of the material's physicochemical properties was conducted using a range of analytical techniques, including, PXRD, nitrogen adsorption-desorption, ammonia TPD, TGA, XPS, FTIR, SEM-EDX, CHN(O) analysis, and ICP-OES. These techniques thoroughly understood the material's structure, composition, and properties. M-MOF 808 AA demonstrated exceptional stability and reusability as a true heterogeneous catalyst, maintaining its activity without any discernible loss over at least four consecutive reaction cycles. A gram-scale conversion was successfully achieved to demonstrate the bulk scalability and industrial potential of the methanol-activated MOF-808 AA catalyst, highlighting its promise for large-scale synthesis and applications.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"582 \",\"pages\":\"Article 115167\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-05-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823125003529\",\"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":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823125003529","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Synthesis and catalytic application of MOF-808 AA as heterogeneous catalyst in catalytic transfer hydrogenation reactions of α-Keto amides
In this study, MOF-808 AA was synthesized by modulating the ratio of DMF to acetic acid, and its catalytic performance was evaluated in the transfer hydrogenation of α-keto amides using isopropanol (IPA) as a green hydrogen source and solvent. Furthermore, the methanol activation method was successfully applied to modify MOF-808 AA, resulting in a significantly enhanced catalyst that surpasses the performance of its pristine counterpart in the catalytic transfer hydrogenation (CTH) of α-keto amides. The catalytic conversion of α-keto amide to α‑hydroxy amide proceeded with remarkable efficiency, yielding 84–99 % conversion within a remarkably brief reaction period of 30 min. This protocol showcased remarkable catalytic versatility, efficiently converting a diverse range of α-keto amides, both activating and deactivating substituents on the aniline ring and benzene rings attached to the keto group. A comprehensive characterization of the material's physicochemical properties was conducted using a range of analytical techniques, including, PXRD, nitrogen adsorption-desorption, ammonia TPD, TGA, XPS, FTIR, SEM-EDX, CHN(O) analysis, and ICP-OES. These techniques thoroughly understood the material's structure, composition, and properties. M-MOF 808 AA demonstrated exceptional stability and reusability as a true heterogeneous catalyst, maintaining its activity without any discernible loss over at least four consecutive reaction cycles. A gram-scale conversion was successfully achieved to demonstrate the bulk scalability and industrial potential of the methanol-activated MOF-808 AA catalyst, highlighting its promise for large-scale synthesis and applications.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods