Metal-organic frameworks (MOFs) have recently received increasing interest due to their potential application in the energy storage and conversion field. Herein, cobalt-based layered MOF ({[Co(Hmt)(tfbdc)(H2O)2]·(H2O)2}n, Co-LMOF; Hmt = hexamethylenetetramine; H2tfbdc = 2,3,5,6-tetrafluoroterephthalic acid) has been evaluated as an electrode material for supercapacitors. The Co-LMOF electrode exhibits a high specific capacitance and excellent cycling stability. Its maximum specific capacitance is 2474 F g(-1) at a current density of 1 A g(-1), and the specific capacitance retention is about 94.3% after 2000 cycles. The excellent electrochemical property may be ascribed to the intrinsic nature of Co-LMOF, enough space available for the storage and diffusion of the electrolyte, and the particles of nanoscale size.
Developing a universal strategy to design piezochromic luminescent materials with desirable properties remains challenging. Here, we report that insertion of a non-emissive molecule into a donor (perylene) and acceptor (1,2,4,5-tetracyanobezene) binary cocrystal can realize fine manipulation of intermolecular interactions between perylene and 1,2,4,5-tetracyanobezene (TCNB) for desirable piezochromic luminescent properties. A continuous pressure-induced emission enhancement up to 3 GPa and a blue shift from 655 to 619 nm have been observed in perylene-TCNB cocrystals upon THF insertion, in contrast to the red-shifted and quenched emission observed when compressing perylene-TCNB cocrystals and other cocrystals reported earlier. By combining experiment with theory, it is further revealed that the inserted non-emissive THF forms blue-shifting hydrogen bonds with neighboring TCNB molecules and promote a conformation change of perylene molecules upon compression, causing the blue-shifted and enhanced emission. This strategy remains valid when inserting other molecules as non-emissive component into perylene-TCNB cocrystals for abnormal piezochromic luminescent behaviors.
A simple metal-free method for the synthesis of 3-aryloxindoles via Brønsted acid catalyzed aromatic C-H functionalization of electron-rich arenes with 3-diazooxindoles is developed. In the presence of a catalytic amount of TfOH, a series of 3-aryloxindoles are synthesized as single regioisomers in good to excellent yields. This transformation is proposed to proceed through acid-catalyzed protonation of 3-diazooxindoles into diazonium ions followed by Friedel-Crafts-type alkylation of arenes.
A new strategy for the synthesis of N-alkoxycarbonyl aryl a-imino esters in the presence of dirhodium tetraacetate [Rh 2 A C H T U N G T R E N N U N G (OAc) 4 ] is reported to produce the desired compounds in high yield (up to 96%) under mild reaction conditions. The application of the synthetic method is demonstrated in enantioselective reduction and Friedel-Crafts reaction of indoles to afford the corresponding chiral arylglycines and indole derivatives, respectively, in high yield and excellent ee.
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