In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small mo...In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules.The interaction between Ni and Co can optimize the electronic structure,resulting in the improved conductivity and accelerated charge transfer rate.The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process.Post-structure and catalytic characterizations confirm the surface oxidation of(Ni,Co)S_(2)during the stability test,and the in-situ formed Co(Ni)based(oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability.As a result,the optimal(Ni,Co)S_(2)solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation,in which a high conversion of benzyl alcohol(97.50%),a good selectivity to benzoic acid(93.78%)and a satisfied faraday efficiency(91.86%)can be achieved.展开更多
This vertically self‐pillared(VSP)structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction kinetics.Here,we prepare a single crystal metal‐organic ...This vertically self‐pillared(VSP)structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction kinetics.Here,we prepare a single crystal metal‐organic framework(MOF),employing the ZIF‐67 structure as a proof of concept,which is constructed by vertically self‐pillared nanosheets(VSP‐MOF).We further converted VSP‐MOF into VSP‐cobalt sulfide(VSP‐CoS2)through a sulfidation process.Catalysis plays an important role in almost all battery technologies;for metallic batteries,lithium anodes exhibit a high theoretical specific capacity,low density,and low redox potential.However,during the half‐cell reaction(Li++e=Li),uncontrolled dendritic Li penetrates the separator and solid electrolyte interphase layer.When employed as a composite scaffold for lithium metal deposition,there are many advantage to using this framework:1)the VSP‐CoS2 substrate provides a high specific surface area to dissipate the ion flux and mass transfer and acts as a pre‐catalyst,2)the catalytic Co center favors the charge transfer process and preferentially binds the Li+with the enhanced electrical fields,and 3)the VSP structure guides the metallic propagation along the nanosheet 2D orientation without the protrusive dendrites.All these features enable the VSP structure in metallic batteries with encouraging performances.展开更多
基金supported by National Natural Science Foundation of China(Nos.21927811,51602182,21808129)the Natural Science Foundation of Shandong Province,China(No.ZR2021ME032)。
文摘In this work,we fabricated an efficient pre-catalyst based on(Ni,Co)S2solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules.The interaction between Ni and Co can optimize the electronic structure,resulting in the improved conductivity and accelerated charge transfer rate.The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process.Post-structure and catalytic characterizations confirm the surface oxidation of(Ni,Co)S_(2)during the stability test,and the in-situ formed Co(Ni)based(oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability.As a result,the optimal(Ni,Co)S_(2)solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation,in which a high conversion of benzyl alcohol(97.50%),a good selectivity to benzoic acid(93.78%)and a satisfied faraday efficiency(91.86%)can be achieved.
文摘This vertically self‐pillared(VSP)structure extends the application range of traditional porous materials with facile mass/ion transport and enhanced reaction kinetics.Here,we prepare a single crystal metal‐organic framework(MOF),employing the ZIF‐67 structure as a proof of concept,which is constructed by vertically self‐pillared nanosheets(VSP‐MOF).We further converted VSP‐MOF into VSP‐cobalt sulfide(VSP‐CoS2)through a sulfidation process.Catalysis plays an important role in almost all battery technologies;for metallic batteries,lithium anodes exhibit a high theoretical specific capacity,low density,and low redox potential.However,during the half‐cell reaction(Li++e=Li),uncontrolled dendritic Li penetrates the separator and solid electrolyte interphase layer.When employed as a composite scaffold for lithium metal deposition,there are many advantage to using this framework:1)the VSP‐CoS2 substrate provides a high specific surface area to dissipate the ion flux and mass transfer and acts as a pre‐catalyst,2)the catalytic Co center favors the charge transfer process and preferentially binds the Li+with the enhanced electrical fields,and 3)the VSP structure guides the metallic propagation along the nanosheet 2D orientation without the protrusive dendrites.All these features enable the VSP structure in metallic batteries with encouraging performances.
