Feng Xuanyu, Song Yang, Chen Justin S, Li Zhe, Chen Emily Y, Kaufmann Michael, Wang Cheng, Lin Wenbin
Department of Chemistry , University of Chicago , 929 E. 57th St. , Chicago , Illinois 60637 , USA . Email:
College of Chemistry and Chemical Engineering , iCHEM , State Key Laboratory of Physical Chemistry of Solid Surface , Xiamen University , Xiamen 361005 , PR China.
Chem Sci. 2018 Dec 19;10(7):2193-2198. doi: 10.1039/c8sc04610g. eCollection 2019 Feb 21.
We report here a novel Ti-BPDC metal-organic framework (MOF) constructed from biphenyl-4,4'-dicarboxylate (BPDC) linkers and Ti(OH) secondary building units (SBUs) with permanent porosity and large 1D channels. Ti-OH groups from neighboring SBUs point toward each other with an O-O distance of 2 Å, and upon deprotonation, act as the first bidentate SBU-based ligands to support Co-hydride species for effective cascade reduction of N-heteroarenes (such as pyridines and quinolines) sequential dearomative hydroboration and hydrogenation, affording piperidine and 1,2,3,4-tetrahydroquinoline derivatives with excellent activity (turnover number ∼ 1980) and chemoselectivity.
我们在此报告一种新型的钛-联苯二甲酸金属有机框架（MOF），它由联苯-4,4'-二羧酸（BPDC）连接体和Ti(OH)二级构筑单元（SBUs）构建而成，具有永久孔隙率和大的一维通道。相邻SBUs中的Ti-OH基团彼此指向，O-O距离为2 Å，去质子化后，作为首个基于二齿SBU的配体，以支持钴氢化物物种对氮杂芳烃（如吡啶和喹啉）进行有效的级联还原——顺序脱芳硼氢化和氢化反应，得到具有优异活性（周转数~1980）和化学选择性的哌啶和1,2,3,4-四氢喹啉衍生物。
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