近日,我校化学化工学院江智勇教授团队在国际化学顶级期刊Nature Chemistry上发表了题为"Leveraging Electron Donor-Acceptor Complexes for Kinetic Resolution in Catalytic Asymmetric Photochemical Synthesis”的研究论文....近日,我校化学化工学院江智勇教授团队在国际化学顶级期刊Nature Chemistry上发表了题为"Leveraging Electron Donor-Acceptor Complexes for Kinetic Resolution in Catalytic Asymmetric Photochemical Synthesis”的研究论文.该研究首次提出了一种基于电子供体-受体(EDA)复合物的动力学拆分策略,成功实现了催化不对称光化学合成.化学化工学院青年教师邵天举博士为论文第一作者,我校学术副校长、化学化工学院院长江智勇教授为唯一通讯作者,河南师范大学为第一通讯单位.展开更多
Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using iso...Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source.The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of(S)-rivastigmine.Building on this success,we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal,nickel.展开更多
Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)...Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)bond construction often rely on expensive and scarce transition metal catalysts,raising concerns about sustainability and environmental impact.To address these challenges,we develop a bifunctional photocatalyst,phloroglucinol carbon quantum dot(PG-CQD).It facilitates catalytic transfer hydrogenation(CTH)with IPA as the hydrogen donor.PG-CQDs exhibit both dehydrogenation and reduction activities,enabling the formation of vicinal diols under mild conditions with visible light irradiation.We propose a CTH mechanism that has been successfully validated through experiments.The catalytic system demonstrates remarkable versatility,enabling the synthesis of various vicinal diols from diverseα-keto ester substrates with good or excellent yields.These findings offer a sustainable synthetic strategy that aligns with green chemistry principles and establish a promising pathway for the development of environmentally benign and energy-efficient organic transformations.展开更多
文摘近日,我校化学化工学院江智勇教授团队在国际化学顶级期刊Nature Chemistry上发表了题为"Leveraging Electron Donor-Acceptor Complexes for Kinetic Resolution in Catalytic Asymmetric Photochemical Synthesis”的研究论文.该研究首次提出了一种基于电子供体-受体(EDA)复合物的动力学拆分策略,成功实现了催化不对称光化学合成.化学化工学院青年教师邵天举博士为论文第一作者,我校学术副校长、化学化工学院院长江智勇教授为唯一通讯作者,河南师范大学为第一通讯单位.
基金supported by the National Natural Science Foundation of China(Nos.22271007,W2431014)Peking University Shenzhen Graduate School+2 种基金State Key Laboratory of Chemical OncogenomicsShenzhen Key Laboratory of Chemical GenomicsShenzhen Bay Laboratory.
文摘Chiral benzylic amines are important motifs in medicines.A dicationic nickel complex of chiral diphosphine(R)-Ph-BPE promotes highly enantioselective reductive amination of aryl alkyl ketones with arylamines using isopropanol as hydrogen source.The reaction is easily scaled up in a gram-scale synthesis using 1 mol% nickel catalyst and it is applied to an asymmetric synthesis of(S)-rivastigmine.Building on this success,we achieved rare examples of asymmetric hydrogen borrowing reactions with arylamines using an Earth-abundant 3d metal,nickel.
基金National Natural Science Foundation of China(Nos.21902023 and 21901252)Shanghai Pujiang Program,China(No.19PJ1400300)+1 种基金Professor of Special Appointment(Eastern Scholar),ChinaShanghai Institutions of Higher Education Fundamental Research Funds for the Central Universities,China(No.0900000155)。
文摘Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)bond construction often rely on expensive and scarce transition metal catalysts,raising concerns about sustainability and environmental impact.To address these challenges,we develop a bifunctional photocatalyst,phloroglucinol carbon quantum dot(PG-CQD).It facilitates catalytic transfer hydrogenation(CTH)with IPA as the hydrogen donor.PG-CQDs exhibit both dehydrogenation and reduction activities,enabling the formation of vicinal diols under mild conditions with visible light irradiation.We propose a CTH mechanism that has been successfully validated through experiments.The catalytic system demonstrates remarkable versatility,enabling the synthesis of various vicinal diols from diverseα-keto ester substrates with good or excellent yields.These findings offer a sustainable synthetic strategy that aligns with green chemistry principles and establish a promising pathway for the development of environmentally benign and energy-efficient organic transformations.
