A new organic-inorganic hybrid based on tungstophosphate anions and benzotria- zole cations, [Na（BTA）E（H2O）2]2[{Cd（BTA）4（H2O）}2（P2W18O62）]·6H2O （1） （BTA = benzotriazole） has been synthesized in aque...A new organic-inorganic hybrid based on tungstophosphate anions and benzotria- zole cations, [Na（BTA）E（H2O）2]2[{Cd（BTA）4（H2O）}2（P2W18O62）]·6H2O （1） （BTA = benzotriazole） has been synthesized in aqueous solution and characterized by elemental analysis, IR spectroscopy, thermal gravimetric analysis, and single-crystal X-ray diffraction. X-ray analysis showed that both {Na（BTA）2} and {Cd（BTA）4} units are supported on the a-Dawson polyoxoanion [P2W18062]6- via the surface bridging oxygen atoms. The electrochemical properties of 1 in aqueous solution are studied at room temperature. It was found that 1 presents good electrocatalytic activities for the reduction of NO2^-.展开更多
Energy storage devices with high volumetric and gravimetric capacitance are in urgent demand due to the booming market of portable and wearable electronics.Using redox-active molecules as electrolytes is a strategy to...Energy storage devices with high volumetric and gravimetric capacitance are in urgent demand due to the booming market of portable and wearable electronics.Using redox-active molecules as electrolytes is a strategy to improve the capacitance and energy density of solid-state supercapacitors(SCs).In this study,polyoxometalates(POMs)are applied as proton conductors and redox mediators in polyvinyl alcohol(PVA)electrolytes,which increase the capacitance of obtained SCs with polyaniline(PANI).H_(3)PMo_(12)O_(40)-loaded PANI electrodes provide pseudocapacitance with an eight-electron Faraday reaction in a charge–discharge cycle.This has rarely been reported in SCs before.The largest capacitance of SCs with H_(3)PMo_(12)O_(40)and H_(3)PW_(12)O_(40)as electrolytes is 7.69 F/cm^(2)(3840 F/g)based on a single electrode at 0.5 mA/cm^(2).In addition,POM electrolytes exhibit excellent self-healing ability,which is attributed to the rich hydrogen-bonding network between POMs and PVA.This study demonstrates that the capacitance of solid-state SCs is improved by using molecular redox-active electrolytes and showcases the potential of applying this strategy to other energy storage devices in the future.展开更多
The nanoreactors were fabricated by reacting amphiphilic quaternary ammoniums and polyoxoperoxometalates Kn[PW12-xTix. O40-x（O2）x] （x = 1, 2 and 3; n =5, 7 and 9） （K5[PW11TiO39（O2）], KT[PWloTi2038（O2）2] and K...The nanoreactors were fabricated by reacting amphiphilic quaternary ammoniums and polyoxoperoxometalates Kn[PW12-xTix. O40-x（O2）x] （x = 1, 2 and 3; n =5, 7 and 9） （K5[PW11TiO39（O2）], KT[PWloTi2038（O2）2] and K9[PW9Ti3O37（O2）3]）. Fourier transform infrared spectroscopy （FT-IR）, transmission electron microscopy （TEM） were used to characterize the resulting samples. This kind of nanocatalysts could promote NH4SCN＇ degradation into simple inorganic compounds such as SO4^2-, HCO3^- and NO3^- only using oxygen as an oxidant under room conditions.展开更多
A series of multivariate metal-organic frameworks(MOFs)with predictable topologies are stepwise constructed from a predesigned versatile hexadecnuclear zirconium cluster.The[Zr_(16)]cluster is constructed from a cente...A series of multivariate metal-organic frameworks(MOFs)with predictable topologies are stepwise constructed from a predesigned versatile hexadecnuclear zirconium cluster.The[Zr_(16)]cluster is constructed from a center classic[Zr_(6)(μ_(3)-OH)_(4)(μ_(3)-O)_(4)(COO)_(4)]cluster and two capped[Zr_(5)(μ_(3)-OH)_(4)(μ2-O)_(4)(HSQA)_(4)(DMF)_(4)](SQA=squaric acid,DMF=dimethylformamide)clusters which have 24 potential coordination sites to link metal ions and four formate groups to be substituted by other organic ligands.Based on this predesigned cluster.展开更多
Novel polyoxometalate(POM)Pickering interfacial catalyst(PIC)was fabricated through loading(NH_(4))_(5)H_(6)PMo_(4)V_(8)O_(40)(PMo_(4)V_(8))on both alkyl and alkyl-amino groups functionalized silica nanoparticles.PMo_...Novel polyoxometalate(POM)Pickering interfacial catalyst(PIC)was fabricated through loading(NH_(4))_(5)H_(6)PMo_(4)V_(8)O_(40)(PMo_(4)V_(8))on both alkyl and alkyl-amino groups functionalized silica nanoparticles.PMo_(4)V_(8)/SiO_(2)(C_(8)/C_(8)NH_(2)with molar ratio as 1:1)PIC system provided a new catalytic model for aerobic conversion of 5-hydroxymethylfurfural(5-HMF),as well as its recovery and product separation in H_(2)O/methyl isobutyl ketone(MIBK)biphase reaction.Balancing the ratio of PMo_(4)V_(8),C_(8)and C_(8)NH_(2)gave rise to variety in hydrophilicity and hydrophobicity for PMo_(4)V_(8)/SiO_(2)(C_(8)/C_(8)NH_(2)),which enhanced the transformation of 5-HMF to 2,5-diformylfuran(DFF)in H_(2)O/MIBK with 73.7%yield at 81.8%conversion than in H_(2)O or MIBK single phase.展开更多
基金the Department of Education of Jilin Province(No.2014349 and 2015431)Science and Technology Bureau of Jilin City(No.20156418)Jilin Institute of Chemical Technology(No.201343 and 2015031)
文摘A new organic-inorganic hybrid based on tungstophosphate anions and benzotria- zole cations, [Na（BTA）E（H2O）2]2[{Cd（BTA）4（H2O）}2（P2W18O62）]·6H2O （1） （BTA = benzotriazole） has been synthesized in aqueous solution and characterized by elemental analysis, IR spectroscopy, thermal gravimetric analysis, and single-crystal X-ray diffraction. X-ray analysis showed that both {Na（BTA）2} and {Cd（BTA）4} units are supported on the a-Dawson polyoxoanion [P2W18062]6- via the surface bridging oxygen atoms. The electrochemical properties of 1 in aqueous solution are studied at room temperature. It was found that 1 presents good electrocatalytic activities for the reduction of NO2^-.
基金support from the National Natural Science Foundation of China(nos.21871042,21471028,and 21673098)。
文摘Energy storage devices with high volumetric and gravimetric capacitance are in urgent demand due to the booming market of portable and wearable electronics.Using redox-active molecules as electrolytes is a strategy to improve the capacitance and energy density of solid-state supercapacitors(SCs).In this study,polyoxometalates(POMs)are applied as proton conductors and redox mediators in polyvinyl alcohol(PVA)electrolytes,which increase the capacitance of obtained SCs with polyaniline(PANI).H_(3)PMo_(12)O_(40)-loaded PANI electrodes provide pseudocapacitance with an eight-electron Faraday reaction in a charge–discharge cycle.This has rarely been reported in SCs before.The largest capacitance of SCs with H_(3)PMo_(12)O_(40)and H_(3)PW_(12)O_(40)as electrolytes is 7.69 F/cm^(2)(3840 F/g)based on a single electrode at 0.5 mA/cm^(2).In addition,POM electrolytes exhibit excellent self-healing ability,which is attributed to the rich hydrogen-bonding network between POMs and PVA.This study demonstrates that the capacitance of solid-state SCs is improved by using molecular redox-active electrolytes and showcases the potential of applying this strategy to other energy storage devices in the future.
基金supported by the National Natural Science Foundation of China(No.51078066)the foundation of Jilin Provincial Environmental Protection Bureau(No.200929)
文摘The nanoreactors were fabricated by reacting amphiphilic quaternary ammoniums and polyoxoperoxometalates Kn[PW12-xTix. O40-x（O2）x] （x = 1, 2 and 3; n =5, 7 and 9） （K5[PW11TiO39（O2）], KT[PWloTi2038（O2）2] and K9[PW9Ti3O37（O2）3]）. Fourier transform infrared spectroscopy （FT-IR）, transmission electron microscopy （TEM） were used to characterize the resulting samples. This kind of nanocatalysts could promote NH4SCN＇ degradation into simple inorganic compounds such as SO4^2-, HCO3^- and NO3^- only using oxygen as an oxidant under room conditions.
基金supported financially by the NSFC of China(nos.21671034 and 21771035).
文摘A series of multivariate metal-organic frameworks(MOFs)with predictable topologies are stepwise constructed from a predesigned versatile hexadecnuclear zirconium cluster.The[Zr_(16)]cluster is constructed from a center classic[Zr_(6)(μ_(3)-OH)_(4)(μ_(3)-O)_(4)(COO)_(4)]cluster and two capped[Zr_(5)(μ_(3)-OH)_(4)(μ2-O)_(4)(HSQA)_(4)(DMF)_(4)](SQA=squaric acid,DMF=dimethylformamide)clusters which have 24 potential coordination sites to link metal ions and four formate groups to be substituted by other organic ligands.Based on this predesigned cluster.
基金supported by National Natural Science Foundation of China(No.51978134)Jilin Provincial Science and Technology Department(No.20210203205SF)。
文摘Novel polyoxometalate(POM)Pickering interfacial catalyst(PIC)was fabricated through loading(NH_(4))_(5)H_(6)PMo_(4)V_(8)O_(40)(PMo_(4)V_(8))on both alkyl and alkyl-amino groups functionalized silica nanoparticles.PMo_(4)V_(8)/SiO_(2)(C_(8)/C_(8)NH_(2)with molar ratio as 1:1)PIC system provided a new catalytic model for aerobic conversion of 5-hydroxymethylfurfural(5-HMF),as well as its recovery and product separation in H_(2)O/methyl isobutyl ketone(MIBK)biphase reaction.Balancing the ratio of PMo_(4)V_(8),C_(8)and C_(8)NH_(2)gave rise to variety in hydrophilicity and hydrophobicity for PMo_(4)V_(8)/SiO_(2)(C_(8)/C_(8)NH_(2)),which enhanced the transformation of 5-HMF to 2,5-diformylfuran(DFF)in H_(2)O/MIBK with 73.7%yield at 81.8%conversion than in H_(2)O or MIBK single phase.
