{"title":"光氧化还原铁催化的氨基烷基化合成位阻手性β-氨基酸。","authors":"Tianze Zhang,Pengwei Gu,Hanmin Huang","doi":"10.1021/jacs.5c12328","DOIUrl":null,"url":null,"abstract":"β-Amino acids represent a vital class of structural motifs in natural products and pharmaceuticals, motivating sustained research efforts in organic synthesis and peptidomimetics. Despite the development of numerous methods for the preparation of β-amino acids, sterically hindered variants continue to pose challenges for their synthesis. In this context, an alternative approach via carboxyalkylation of prevalent tertiary amine scaffolds offers a promising yet underexplored strategy for the streamlined synthesis of β-amino acid derivatives. Herein, we report the development of an iron-porphyrin/photoredox dual catalytic system for the C(sp3)-C(sp3) cross-coupling of tertiary amines and α-halo acyl compounds, enabling the efficient assembly of sterically hindered β-amino acid frameworks. Mechanistic studies disclosed that the iron catalyst participates in the single-electron oxidation with α-carbonyl radical to generate a ferric enolate intermediate, thereby facilitating Mannich-type addition to afford the desired β-amino acid derivatives. Furthermore, the utilization of chiral auxiliaries enabled efficient stereocontrol over the aminoalkylation process, providing a platform for synthesizing a broad array of chiral β-amino acid derivatives.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"71 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photoredox Fe-Catalyzed Aminoalkylation toward Sterically Hindered Chiral β-Amino Acids.\",\"authors\":\"Tianze Zhang,Pengwei Gu,Hanmin Huang\",\"doi\":\"10.1021/jacs.5c12328\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"β-Amino acids represent a vital class of structural motifs in natural products and pharmaceuticals, motivating sustained research efforts in organic synthesis and peptidomimetics. Despite the development of numerous methods for the preparation of β-amino acids, sterically hindered variants continue to pose challenges for their synthesis. In this context, an alternative approach via carboxyalkylation of prevalent tertiary amine scaffolds offers a promising yet underexplored strategy for the streamlined synthesis of β-amino acid derivatives. Herein, we report the development of an iron-porphyrin/photoredox dual catalytic system for the C(sp3)-C(sp3) cross-coupling of tertiary amines and α-halo acyl compounds, enabling the efficient assembly of sterically hindered β-amino acid frameworks. Mechanistic studies disclosed that the iron catalyst participates in the single-electron oxidation with α-carbonyl radical to generate a ferric enolate intermediate, thereby facilitating Mannich-type addition to afford the desired β-amino acid derivatives. Furthermore, the utilization of chiral auxiliaries enabled efficient stereocontrol over the aminoalkylation process, providing a platform for synthesizing a broad array of chiral β-amino acid derivatives.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"71 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.5c12328\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.5c12328","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
β-Amino acids represent a vital class of structural motifs in natural products and pharmaceuticals, motivating sustained research efforts in organic synthesis and peptidomimetics. Despite the development of numerous methods for the preparation of β-amino acids, sterically hindered variants continue to pose challenges for their synthesis. In this context, an alternative approach via carboxyalkylation of prevalent tertiary amine scaffolds offers a promising yet underexplored strategy for the streamlined synthesis of β-amino acid derivatives. Herein, we report the development of an iron-porphyrin/photoredox dual catalytic system for the C(sp3)-C(sp3) cross-coupling of tertiary amines and α-halo acyl compounds, enabling the efficient assembly of sterically hindered β-amino acid frameworks. Mechanistic studies disclosed that the iron catalyst participates in the single-electron oxidation with α-carbonyl radical to generate a ferric enolate intermediate, thereby facilitating Mannich-type addition to afford the desired β-amino acid derivatives. Furthermore, the utilization of chiral auxiliaries enabled efficient stereocontrol over the aminoalkylation process, providing a platform for synthesizing a broad array of chiral β-amino acid derivatives.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.