Rapidly deactivation of Cu/SiO2 catalysts at high liquid hour space velocity(LHSV) has been an important obstacle for scale-up application.Herein,silver modified copper phyllosilicate nanotubes were fabricated by diff...Rapidly deactivation of Cu/SiO2 catalysts at high liquid hour space velocity(LHSV) has been an important obstacle for scale-up application.Herein,silver modified copper phyllosilicate nanotubes were fabricated by different strategies,and implemented to the selective hydrogenation of ethylene carbonate(EC) to methanol and ethylene glycol(EG) as alternative route for the indirect utilization of CO2.The CuPs Ag-copre catalyst synthesized by the co-ammonia evaporation hydrothermal process achieved79% methanol and 99% EG yield within various ranges of EC LHSV,which was attributed to the balanced Cu+/CuO ratio and the enhanced H2 dissociation ability.Inlaid silver species over copper phyllosilicate promoted the interaction between the metal and the support,which substantially regulated the reducibility and dispersion of copper species,meanwhile,increased the stability for long-term running of the catalyst.展开更多
Construction of metal-organic-frame works-based composite photocatalysts has attracted much attention for the reasonable band gap and high surface areas to improve the photocatalytic activity.In this study,the ternary...Construction of metal-organic-frame works-based composite photocatalysts has attracted much attention for the reasonable band gap and high surface areas to improve the photocatalytic activity.In this study,the ternary heterojunction Pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)nanocomposites were facilely prepared for the first time by a two-step method.The visible-light-promoted hydrogen production rate of 0.3%Pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)reaches up to 5.26 mmol g^(-1)h^(-1),which is evidently much higher than pure UiO-66-NH_(2),ZnIn_(2)S_(4)and binary UiO-66-NH_(2)/ZnIn_(2)S_(4)composites.Such a huge improvement in the photocatalytic performance is mainly attributed to the matched band gap of ZnIn_(2)S_(4)and UiO-66-NH_(2),and the introduction of Pd NPs into photocatalysts that broaden spectral response range and promote the photon induced charge carrier separation.This work may provide a feasible approach for the design and construction of metal-organic-frameworks-based photocatalytic materials.展开更多
Metallic Ni bridged Ni S@mesoporous carbon nitride hybrids were for the first time fabricated through a one-pot electroless-assisted hydrothermal method.The intimate Ni bridge between the interface of mesoporous carbo...Metallic Ni bridged Ni S@mesoporous carbon nitride hybrids were for the first time fabricated through a one-pot electroless-assisted hydrothermal method.The intimate Ni bridge between the interface of mesoporous carbon nitride and Ni S was confirmed by HRTEM and in-depth XPS analysis using an Ar+-cluster sputtering gun and a possible mechanism was put forward to elucidate the formation process of the unique structure.Without adding any noble metals as cocatalysts,the optimized catalyst 10%NiS/mCN-160-12 showed a H2 evolution rate of 1419μmol·g^-1·h^-1,which is about 34 and 14 fold higher than that of bare mesoporous carbon nitride and Ni S,respectively.The dramatically enhanced photocatalytic performance was mainly ascribed to the synergistic effect of Ni S cocatalyst loading and the formation of metallic Ni between the interface of mesoporous carbon nitride and Ni S,which served as a charge-transfer bridge to facilitate the transfer and separation of photo-induced electron-hole pairs.展开更多
基金financially supported by the Natural Science Foundation of Shanghai(19ZR1403500)National Natural Science Foundation of China(No.21373054)the Natural Science Foundation of Shanghai Science and Technology Committee(No.08DZ2270500)。
文摘Rapidly deactivation of Cu/SiO2 catalysts at high liquid hour space velocity(LHSV) has been an important obstacle for scale-up application.Herein,silver modified copper phyllosilicate nanotubes were fabricated by different strategies,and implemented to the selective hydrogenation of ethylene carbonate(EC) to methanol and ethylene glycol(EG) as alternative route for the indirect utilization of CO2.The CuPs Ag-copre catalyst synthesized by the co-ammonia evaporation hydrothermal process achieved79% methanol and 99% EG yield within various ranges of EC LHSV,which was attributed to the balanced Cu+/CuO ratio and the enhanced H2 dissociation ability.Inlaid silver species over copper phyllosilicate promoted the interaction between the metal and the support,which substantially regulated the reducibility and dispersion of copper species,meanwhile,increased the stability for long-term running of the catalyst.
基金the Natural Science Foundation of Shanghai(No.19ZR1403500)the National Natural Science Foundation of China(No.21373054)the Natural Science Foundation of Shanghai Science and Technology Committee(No.19DZ2270100)。
文摘Construction of metal-organic-frame works-based composite photocatalysts has attracted much attention for the reasonable band gap and high surface areas to improve the photocatalytic activity.In this study,the ternary heterojunction Pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)nanocomposites were facilely prepared for the first time by a two-step method.The visible-light-promoted hydrogen production rate of 0.3%Pd@UiO-66-NH_(2)@ZnIn_(2)S_(4)reaches up to 5.26 mmol g^(-1)h^(-1),which is evidently much higher than pure UiO-66-NH_(2),ZnIn_(2)S_(4)and binary UiO-66-NH_(2)/ZnIn_(2)S_(4)composites.Such a huge improvement in the photocatalytic performance is mainly attributed to the matched band gap of ZnIn_(2)S_(4)and UiO-66-NH_(2),and the introduction of Pd NPs into photocatalysts that broaden spectral response range and promote the photon induced charge carrier separation.This work may provide a feasible approach for the design and construction of metal-organic-frameworks-based photocatalytic materials.
基金financial support of the project from the National Natural Science Foundation of Shanghai(19ZR1403500)NNSFC(Project 21373054)the Natural Science Foundation of Shanghai Science and Technology Committee(19DZ2270100)。
文摘Metallic Ni bridged Ni S@mesoporous carbon nitride hybrids were for the first time fabricated through a one-pot electroless-assisted hydrothermal method.The intimate Ni bridge between the interface of mesoporous carbon nitride and Ni S was confirmed by HRTEM and in-depth XPS analysis using an Ar+-cluster sputtering gun and a possible mechanism was put forward to elucidate the formation process of the unique structure.Without adding any noble metals as cocatalysts,the optimized catalyst 10%NiS/mCN-160-12 showed a H2 evolution rate of 1419μmol·g^-1·h^-1,which is about 34 and 14 fold higher than that of bare mesoporous carbon nitride and Ni S,respectively.The dramatically enhanced photocatalytic performance was mainly ascribed to the synergistic effect of Ni S cocatalyst loading and the formation of metallic Ni between the interface of mesoporous carbon nitride and Ni S,which served as a charge-transfer bridge to facilitate the transfer and separation of photo-induced electron-hole pairs.
