化学
立体专一性
金属
铜
高分子化学
立体化学
计算化学
有机化学
催化作用
作者
Debesh Sharma,Sagarmani Rasaily,Shivanand Chettri,Disha Sureka,Sudarsan Tamang,Anand Pariyar
标识
DOI:10.1021/acs.inorgchem.2c04443
摘要
The role of coordinatively unsaturated sites (CUS) in metal–organic framework (MOF)-catalyzed organic transformation is vital; however, the design and generation of such sites are challenging. We, therefore, report the synthesis of a novel two-dimensional (2D) MOF, [Cu(BTC)(Mim)]n (Cu-SKU-3), with pre-existing unsaturated Lewis acid sites. The presence of these active CUS facilitates a ready-to-use attribute in Cu-SKU-3, thereby subsiding the lengthy activation processes associated with MOF-based catalysis. The material has been completely characterized using single crystal X-ray diffraction (SCXRD), powder XRD (PXRD), thermogravimetric analysis (TGA), carbon, hydrogen, and nitrogen (CHN), Fourier-transform infrared (FTIR), and Brunauer–Emmett–Teller (BET) surface area analyses. We directly utilize Cu-SKU-3 for the synthesis of biologically valued chiral imidazolidine motifs in a one-pot fashion starting from aziridines. The chiral imidazolidines are synthesized in good yield (up to 89%) and with high optical purity (ee > 98–99%). Mechanistically, the transformation proceeds in a tandem fashion through stereospecific ring-opening of aziridines followed by the intramolecular cyclization (via sp3 C–H functionalization) reaction forming chiral imidazolidines. The material has an excellent heterogeneous attribute and can be reused several times for one-pot catalytic cycles.
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