The exploration of highly efficient catalysts for the hydrolysis of hydrous hydrazine is of great significance for the achievement of future hydrogen economy.In this regard,herein,a catalyst with NiFePd loaded on the ...The exploration of highly efficient catalysts for the hydrolysis of hydrous hydrazine is of great significance for the achievement of future hydrogen economy.In this regard,herein,a catalyst with NiFePd loaded on the metal-organic framework(MOF)UiO-66 was successfully prepared by a simple and safe chemical impregnation method.Due to its high specific surface area,the as-prepared NiFePd/UiO-66 catalyst exhibited efficient catalytic performance for the generation of hydrogen from hydrous hydrazine in an alkaline solution.The results showed that the Ni_(0.25)Fe_(0.25)Pd_(0.5)/UiO-66 catalyst exhibited optimal properties for the decomposition of hydrous hydrazine in an alkaline aqueous solution with a nearly 100%hydrogen selectivity,good activity,and the high total turnover frequency(TOF)value of up to 662.4 h-1 at 80℃.Moreover,the Ni_(0.25)Fe_(0.25)Pd_(0.5)/UiO-66 catalyst exhibited good durability,which slightly decreased after five cycles of catalytic reaction at 60℃.展开更多
Manganese-based organic metal halides,due to their excellent optoelectronic properties and stable chemical nature,have been widely used in optoelectronic devices and sensors.In this study,through rational modulation o...Manganese-based organic metal halides,due to their excellent optoelectronic properties and stable chemical nature,have been widely used in optoelectronic devices and sensors.In this study,through rational modulation of halogens,three novel zero-dimensional organic manganese halides[(C_(6)H_(8)N)_(2)MnX_(4)(X=Cl,Br,and I)]were obtained by changing the halogen atom via the solvent evaporation method.Due to the d–d electronic transition of Mn^(2+) in the tetrahedrally coordinated[MnX4]^(2−)polyhedron,all samples exhibit strong green emission.Notably,(C_(6)H_(8)N)_(2)MnBr_(4) exhibited a remarkable light yield of 18224 photons per MeV and a low detection limit of 1.9μGy s^(−1),which is below the X-ray diagnostic limit and even superior to that of commercial BGO scintillators.Moreover,a 9 cm×9 cm flexible scintillator film was successfully fabricated by mixing(C_(6)H_(8)N)_(2)MnBr_(4) crystalline powder with polymethyl methacrylate,and this film manifested superior radiation stability and an X-ray imaging resolution of 12.1 lp mm^(−1).Notably,the X-ray images captured by the flexible film demonstrate distinguished clarity when adhered perfectly to curved metal sheets.The combination of excellent performance and facile solution processing opens new opportunities for low-cost,high-performance organic metal halide-based large-area flexible scintillators for X-ray detection and imaging.展开更多
Interfacial charge recombination is a serious problem in semiconductor-sensitized solar cells which severely limits the power conversion efficiency.Herein,an ultrathin SiO_(2)blocking layer was introduced to the TiO_(...Interfacial charge recombination is a serious problem in semiconductor-sensitized solar cells which severely limits the power conversion efficiency.Herein,an ultrathin SiO_(2)blocking layer was introduced to the TiO_(2)surface to suppress the interfacial recombination in Sb_(2)S_(3)-sensitized solar cells.The SiO_(2)blocking layer was deposited by a simple chemical bath method.Due to the unique features of the SiO_(2)layer,the Sb_(2)S_(3)sensitizer shows a remarkable change in the morphology after SiO_(2)coating,forming numerous irregular large crystals which did not bring a negative impact.Electrochemical impedance spectra and opencircuit voltage-decay analysis confirm that the SiO_(2)layer efficiently suppresses the interfacial recombination at the TiO_(2)/Sb_(2)S_(3)interface which is the major recombination path in the solar cells.As a result,the device exhibits remarkably enhanced open-circuit voltage,fill factor and power conversion efficiency.展开更多
A 3D microporous MOF[Cu_(1.5)(BTB-NH_(2))(H_(2)O)_(2)]·6DMA·5H_(2)O(UPC-99)of the(2,3,4-c)-net novel topology type was successfully constructed by the amino-functionalized ligand and Cu(II)ions via a solvoth...A 3D microporous MOF[Cu_(1.5)(BTB-NH_(2))(H_(2)O)_(2)]·6DMA·5H_(2)O(UPC-99)of the(2,3,4-c)-net novel topology type was successfully constructed by the amino-functionalized ligand and Cu(II)ions via a solvothermal method.Due to the presence of two channels with open Cu(II)sites and–NH_(2)groups,UPC-99 exhibits a high adsorption selectivity of 15.3 for CO_(2)/CH_(4)at 1 bar and 273 K.Remarkably,UPC-99 exhibits a significant adsorption difference in C_(3)H_(6) and C_(3)H_(8) relative to CH_(4) and shows a high separation selectivity for C3 light hydrocarbons relative to CH_(4)(496.7 for C_(3)H_(6)/CH_(4)and 410.5 for C_(3)H_(8)/CH_(4) at 273 K,1 bar)by single-component gas sorption and selectivity calculations in IAST methods.Moreover,the presence of open Lewis acidic Cu(II)sites in the channels allows UPC-99 to exhibit excellent catalytic performance in the catalytic cycloaddition reactions of CO_(2)with epoxides.展开更多
基金supported by the National Natural Science Foundation of China(No.51602293 and No.1705168)the Open Project of State Key Laboratory of Environment-friendly Energy Materials(No.18kfhg06).
文摘The exploration of highly efficient catalysts for the hydrolysis of hydrous hydrazine is of great significance for the achievement of future hydrogen economy.In this regard,herein,a catalyst with NiFePd loaded on the metal-organic framework(MOF)UiO-66 was successfully prepared by a simple and safe chemical impregnation method.Due to its high specific surface area,the as-prepared NiFePd/UiO-66 catalyst exhibited efficient catalytic performance for the generation of hydrogen from hydrous hydrazine in an alkaline solution.The results showed that the Ni_(0.25)Fe_(0.25)Pd_(0.5)/UiO-66 catalyst exhibited optimal properties for the decomposition of hydrous hydrazine in an alkaline aqueous solution with a nearly 100%hydrogen selectivity,good activity,and the high total turnover frequency(TOF)value of up to 662.4 h-1 at 80℃.Moreover,the Ni_(0.25)Fe_(0.25)Pd_(0.5)/UiO-66 catalyst exhibited good durability,which slightly decreased after five cycles of catalytic reaction at 60℃.
基金financial support from the National Natural Science Foundation of China(Grant No.62305195)the projects ZR2024ME223 and ZR2022QF036 supported by the Shandong Provincial Natural Science Foundationthe Opening Project of State Key Laboratory of Crystal Materials(Shandong University,KF2105).
文摘Manganese-based organic metal halides,due to their excellent optoelectronic properties and stable chemical nature,have been widely used in optoelectronic devices and sensors.In this study,through rational modulation of halogens,three novel zero-dimensional organic manganese halides[(C_(6)H_(8)N)_(2)MnX_(4)(X=Cl,Br,and I)]were obtained by changing the halogen atom via the solvent evaporation method.Due to the d–d electronic transition of Mn^(2+) in the tetrahedrally coordinated[MnX4]^(2−)polyhedron,all samples exhibit strong green emission.Notably,(C_(6)H_(8)N)_(2)MnBr_(4) exhibited a remarkable light yield of 18224 photons per MeV and a low detection limit of 1.9μGy s^(−1),which is below the X-ray diagnostic limit and even superior to that of commercial BGO scintillators.Moreover,a 9 cm×9 cm flexible scintillator film was successfully fabricated by mixing(C_(6)H_(8)N)_(2)MnBr_(4) crystalline powder with polymethyl methacrylate,and this film manifested superior radiation stability and an X-ray imaging resolution of 12.1 lp mm^(−1).Notably,the X-ray images captured by the flexible film demonstrate distinguished clarity when adhered perfectly to curved metal sheets.The combination of excellent performance and facile solution processing opens new opportunities for low-cost,high-performance organic metal halide-based large-area flexible scintillators for X-ray detection and imaging.
基金supported by the Distinguished Youth Foundation of Anhui Province(1708085J09)the National Basic Research Program of China under Grant No.2015CB932200+1 种基金the National Natural Science Foundation of China under Grant No.21403247the Major/Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology(2016FXZY003).
文摘Interfacial charge recombination is a serious problem in semiconductor-sensitized solar cells which severely limits the power conversion efficiency.Herein,an ultrathin SiO_(2)blocking layer was introduced to the TiO_(2)surface to suppress the interfacial recombination in Sb_(2)S_(3)-sensitized solar cells.The SiO_(2)blocking layer was deposited by a simple chemical bath method.Due to the unique features of the SiO_(2)layer,the Sb_(2)S_(3)sensitizer shows a remarkable change in the morphology after SiO_(2)coating,forming numerous irregular large crystals which did not bring a negative impact.Electrochemical impedance spectra and opencircuit voltage-decay analysis confirm that the SiO_(2)layer efficiently suppresses the interfacial recombination at the TiO_(2)/Sb_(2)S_(3)interface which is the major recombination path in the solar cells.As a result,the device exhibits remarkably enhanced open-circuit voltage,fill factor and power conversion efficiency.
基金supported by the National Natural Science Foundation of China(NSFC,Grant No.21771191,21571187)the Taishan Scholar Foundation(ts201511019)+1 种基金the Shandong Natural Science Fund(ZR2017QB012)the Fundamental Research Funds for the Central Universities(18CX06003A,YCX2018071).
文摘A 3D microporous MOF[Cu_(1.5)(BTB-NH_(2))(H_(2)O)_(2)]·6DMA·5H_(2)O(UPC-99)of the(2,3,4-c)-net novel topology type was successfully constructed by the amino-functionalized ligand and Cu(II)ions via a solvothermal method.Due to the presence of two channels with open Cu(II)sites and–NH_(2)groups,UPC-99 exhibits a high adsorption selectivity of 15.3 for CO_(2)/CH_(4)at 1 bar and 273 K.Remarkably,UPC-99 exhibits a significant adsorption difference in C_(3)H_(6) and C_(3)H_(8) relative to CH_(4) and shows a high separation selectivity for C3 light hydrocarbons relative to CH_(4)(496.7 for C_(3)H_(6)/CH_(4)and 410.5 for C_(3)H_(8)/CH_(4) at 273 K,1 bar)by single-component gas sorption and selectivity calculations in IAST methods.Moreover,the presence of open Lewis acidic Cu(II)sites in the channels allows UPC-99 to exhibit excellent catalytic performance in the catalytic cycloaddition reactions of CO_(2)with epoxides.
