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
Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))an...Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))and unraveling its structure−activity relationship.By leveraging transition molybdenum polysulfide clusters as functional units for multi-level ordering,we successfully designed and synthesized MoS_(x)nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters via evaporationinduced self-assembly,which exhibit enhanced HER activity attributed to a high density of active sites and dynamic evolution behavior under cathodic potentials.MoS_(x) nanowire networks electrode yields a current density of 100 mA·cm^(−2) at 142 mV in 0.5 M H_(2)SO_(4).This work provides an attractive prospect for optimizing catalysts at the sub-nano scale and offers insights into a strategy for designing catalysts in various gas evolution reactions.展开更多
Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance a...Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance are still a challenge.Herein,NH_(4)^(+)and glycerate anions pre-inserted Mo glycerate(N-MoG)spheres are synthesized and serve as the template to form NH_(4)^(+)intercalated Ni_(3)S_(2)/Ni_(3)O_(2)(OH)_(4)@MoS_(2)core–shell nanoflower(N-NiMo-OS)in-situ grown on nickel foam(NF)(N-NiMo-OS/NF)by sulfurization treatment.Compared with the product using traditional MoG as a template,N-NiMo-OS/NF inheriting a larger core structure from N-MoG delivers enhanced space for ions transport and volume expansion during the energy storage process,together with the synergistic effects of multi-components and the heterostructure,the as-prepared N-NiMo-OS/NF nanoflower exhibits excellent performance for the battery-type hybrid supercapacitors(BHS)and ZHS devices.Notably,the ZHS device delivers superior electrochemical performance to the BHS device,such as a higher specific capacity of 327.5 mAh·g^(−1)at 1 A·g^(−1),a preeminent energy density of 610.6 Wh·kg^(−1)at 1710 W·kg^(−1),long cycle life.The in-situ Raman,ex-situ X-ray photoelectron spectroscopy(XPS),theoretical calculation demonstrate the extra Zn^(2+)insertion/extraction storage mechanism provides enhanced electrochemical performance for ZHS device.Therefore,the dual-ion pre-inserted strategy can be extended for other advanced electrode materials in energy storage fields.展开更多
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.
基金supported by Innovation Support Programme(Soft Science Research)Project Achievements of Jiangsu Province(No.BK20231514)the National College Student Innovation and Entrepreneurship Training Program(NO.202310293173K).
文摘Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))and unraveling its structure−activity relationship.By leveraging transition molybdenum polysulfide clusters as functional units for multi-level ordering,we successfully designed and synthesized MoS_(x)nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters via evaporationinduced self-assembly,which exhibit enhanced HER activity attributed to a high density of active sites and dynamic evolution behavior under cathodic potentials.MoS_(x) nanowire networks electrode yields a current density of 100 mA·cm^(−2) at 142 mV in 0.5 M H_(2)SO_(4).This work provides an attractive prospect for optimizing catalysts at the sub-nano scale and offers insights into a strategy for designing catalysts in various gas evolution reactions.
基金the National Natural Science Foundation of China(Nos.21702116,51772162,and 52072197)the 111 Project of China(No.D20017)+5 种基金Shandong Provincial Key Research and Development Program,China(No.2019GSF107087)Qingdao Postdoctoral Sustentation Fund,Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)Taishan Scholar Young Talent Program(No.tsqn201909114)Major Scientific and Technological Innovation Project(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09).
文摘Zinc ion hybrid supercapacitors(ZHS)have received much attention due to the enhanced potential window range and high specific capacity.However,the appropriate positive materials with high electrochemical performance are still a challenge.Herein,NH_(4)^(+)and glycerate anions pre-inserted Mo glycerate(N-MoG)spheres are synthesized and serve as the template to form NH_(4)^(+)intercalated Ni_(3)S_(2)/Ni_(3)O_(2)(OH)_(4)@MoS_(2)core–shell nanoflower(N-NiMo-OS)in-situ grown on nickel foam(NF)(N-NiMo-OS/NF)by sulfurization treatment.Compared with the product using traditional MoG as a template,N-NiMo-OS/NF inheriting a larger core structure from N-MoG delivers enhanced space for ions transport and volume expansion during the energy storage process,together with the synergistic effects of multi-components and the heterostructure,the as-prepared N-NiMo-OS/NF nanoflower exhibits excellent performance for the battery-type hybrid supercapacitors(BHS)and ZHS devices.Notably,the ZHS device delivers superior electrochemical performance to the BHS device,such as a higher specific capacity of 327.5 mAh·g^(−1)at 1 A·g^(−1),a preeminent energy density of 610.6 Wh·kg^(−1)at 1710 W·kg^(−1),long cycle life.The in-situ Raman,ex-situ X-ray photoelectron spectroscopy(XPS),theoretical calculation demonstrate the extra Zn^(2+)insertion/extraction storage mechanism provides enhanced electrochemical performance for ZHS device.Therefore,the dual-ion pre-inserted strategy can be extended for other advanced electrode materials in energy storage fields.
