CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based c...CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.展开更多
Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS_(2),we unlock the potential of Mo sites and successfully prepared novel MoS_(2)@Ni_(3)S_(2)/NF core-shell nanospheres a...Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS_(2),we unlock the potential of Mo sites and successfully prepared novel MoS_(2)@Ni_(3)S_(2)/NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction(HER).TheΔGH at the Mo site is optimized via Ni_(3)S_(2)to achieve excellent HER activity.At low current densities,it has similar activity to the Pt/C.However,its performance is better than Pt/C at high density.Moreover,our catalyst shows a considerable stability at a variety of current densities for 50 h,promising to substitute noble metal catalysts in application of commercial alkaline electrocatalysts.展开更多
文摘CO_(2)hydrogenation to value-added light olefins(C_(2-4)=)is crucial for the utilization and cycling of global carbon resource.Moderate CO_(2)activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO_(2)conversion to target C_(2-4)=products.The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance.Here,we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method.The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phaseχ-(Fe_(x)Co_(1-x))_(5)C_(2)and improves CO_(2)adsorption capacity,enhancing the efficient conversion of CO_(2)and moderate C-C coupling.Therefore,the catalyst FeCoK@C exhibits C_(2-4)=selectivity of 33.0%while maintaining high CO_(2)conversion of 52.0%.The high stability without obvious deactivation for over 100 h and unprecedented C_(2-4)=space time yield(STY)up to 52.9 mmolCO_(2)·g^(-1)·h^(-1)demonstrate its potential for practical application.This work provides an efficient strategy for the development of high-performance CO_(2)hydrogenation catalysts.
基金supported by the National Natural Science Foundation of China(grant Nos.51872115,52101256)the Project funded by China Postdoctoral Science Foundation(grant No.2020M680043)+1 种基金Science and Technology Research Project of the Department of Educationof JilinProvince(grant No.JKH20211083KJ)2020 INTERNATIONAL COOPERATION Project of the Department of Science and Technology of Jjilin Province(grant No.20200801001GH).
文摘Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS_(2),we unlock the potential of Mo sites and successfully prepared novel MoS_(2)@Ni_(3)S_(2)/NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction(HER).TheΔGH at the Mo site is optimized via Ni_(3)S_(2)to achieve excellent HER activity.At low current densities,it has similar activity to the Pt/C.However,its performance is better than Pt/C at high density.Moreover,our catalyst shows a considerable stability at a variety of current densities for 50 h,promising to substitute noble metal catalysts in application of commercial alkaline electrocatalysts.
