Metal-organic frameworks(MOFs)functionalized with open metal sites(OMSs)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest mole...Metal-organic frameworks(MOFs)functionalized with open metal sites(OMSs)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest molecules.However,rational tailoring of the coordination environment of metal nodes dur-ing the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with linkers.Herein,we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ)sites,namely[Cu(HCOO)(pzta)]_(n)(HL-1),{[Cu(PTA)0.5(pzta)(H_(2)O)]·2H_(2)O}_(n)(HL-2)and[Cu(NA)0.5(pzta)]_(n)(HL-3)(Hpzta=3-pyrazinyl-1,2,4-triazole;PTA=terephthalic acid;NA=1,4-naphthalene dicarboxylic acid),based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ligands.Re-markably,the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions(25℃and 1 atm).In particular,the complete conversion of 4-nitrophenol(4-NP)took only 30 s on HL-2,reaching a record-high TOF value compared with previously reported metal catalysts.The combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron trans-port between the substrates,and was responsible for the outstanding performance.This work shined lights on the further enhancement of performance for MOFs through rational OMSs construction.展开更多
Series of novel derivatives of desloratadine designed as arginine vasopressin receptor antagonists were synthesized and structurally characterized by melting points,^1H NMR and HRMS.Their in vivo diuretic activities w...Series of novel derivatives of desloratadine designed as arginine vasopressin receptor antagonists were synthesized and structurally characterized by melting points,^1H NMR and HRMS.Their in vivo diuretic activities were evaluated on rats,and several target compounds showed promising diuretic results, especially compounds 8,18,27 and 31.Further in vitro bonding assay and cAMP assay showed that these compounds had a higher affinity to vasopressin V2 receptor than VI a receptor.Our studies indicated that desloratadine may be an active substructure for novel arginine vasopressin receptor antagonist development.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21902022,81903501,21601028)Qingchuang Science and Technology Plan of Shandong Province(No.2021KJ054)+1 种基金the Natural Science Foundation of Shandong Province(Nos.ZR2018LB018,ZR2019QB026,ZR2022QB058,ZR2020KB014)Scientific Research Foundation of Dezhou University(Nos.30101905,30102708,30102701).
文摘Metal-organic frameworks(MOFs)functionalized with open metal sites(OMSs)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest molecules.However,rational tailoring of the coordination environment of metal nodes dur-ing the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with linkers.Herein,we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ)sites,namely[Cu(HCOO)(pzta)]_(n)(HL-1),{[Cu(PTA)0.5(pzta)(H_(2)O)]·2H_(2)O}_(n)(HL-2)and[Cu(NA)0.5(pzta)]_(n)(HL-3)(Hpzta=3-pyrazinyl-1,2,4-triazole;PTA=terephthalic acid;NA=1,4-naphthalene dicarboxylic acid),based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ligands.Re-markably,the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions(25℃and 1 atm).In particular,the complete conversion of 4-nitrophenol(4-NP)took only 30 s on HL-2,reaching a record-high TOF value compared with previously reported metal catalysts.The combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron trans-port between the substrates,and was responsible for the outstanding performance.This work shined lights on the further enhancement of performance for MOFs through rational OMSs construction.
基金project was supported by National 973 Plan(Nos. 2010CB735602 and 2012CB724002)National Major Scientific and Technological Special Project for "Significant New Drugs Development"(No.2011ZX09401-009)
文摘Series of novel derivatives of desloratadine designed as arginine vasopressin receptor antagonists were synthesized and structurally characterized by melting points,^1H NMR and HRMS.Their in vivo diuretic activities were evaluated on rats,and several target compounds showed promising diuretic results, especially compounds 8,18,27 and 31.Further in vitro bonding assay and cAMP assay showed that these compounds had a higher affinity to vasopressin V2 receptor than VI a receptor.Our studies indicated that desloratadine may be an active substructure for novel arginine vasopressin receptor antagonist development.
