Two-dimensional (2D)Ni(OH)_(2) nanosheets can theoretically expose their active sites of 100%.Whereas,their intrinsic easy accumulation and low conductivity lead to weak and unsustainable reaction kinetics.Herein,we p...Two-dimensional (2D)Ni(OH)_(2) nanosheets can theoretically expose their active sites of 100%.Whereas,their intrinsic easy accumulation and low conductivity lead to weak and unsustainable reaction kinetics.Herein,we propose a novel halogen chlorine-triggered electrochemical etching strategy to controllably manage the reaction kinetics of 2D Ni(OH)_(2) nanosheets(EE/Cl-Ni(OH)_(2)).It is found that halogen chlorine doping can adjust the interlamellar spacing flexibly and promote the lattice oxygen activation to achieve controlled construction of superficial oxygen defects at the adjustable voltage.The optimal EE/Cl-Ni(OH)_(2) electrode exhibits a high rate capability and excellent specific capacity of 206.9 mA h g^(-1) at 1 A g^(-1) in a three-electrode system,which is more than twice as high as the pristine Ni(OH)_(2).Furthermore,EE/Cl-Ni(OH)_(2) cathode and FeOOH@rGO anode are employed for developing an aqueous Ni-Fe battery with an excellent energy density of 83 W h kg^(-1),a high power density of 17051 W kg^(-1),and robust durability over 20,000 cycles.This strategy exploits a fresh channel for the ingenious fabrication of highefficiency and stable nickel-based deficiency materials for energy storage.展开更多
lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synt...lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synthesized by a low-temperature hydrothermal method using a tai-lored diquaternary ammonium surfactant as the structure-directing agent.Introducing Ni^2+cationsat the ion-exchange sites of the TS-1 NS framework significantly enhanced its photoactivity in aero-bic alcohol oxidation.The optimized Ni cation-functionalized TS-1 NS(Ni/TS-1 NS)provide impres-sive photoactivity,with a benzyl alcohol(BA)conversion of 78.9%and benzyl aldehyde(BAD)se-lectivity of 98.8%using O as the only oxidant under full light irradiation;this BAD yield is approx-imately six times greater than that obtained for bulk TS-1,and is maintained for five runs.The ex-cellent photoactivity of Ni/TS-1 NS is attributed to the significantly enlarged surface area of thetwo-dimensional morphology TS-1 NS,extra mesopores,and greatly improved charge separation.Compared with bulk TS-1,Ni/TS-1 NS has a much shorter charge transfer distance.Theas-introduced Ni species could capture the photoelectrons to further improve the charge separa-tion.This work opens the way to a class of highly selective,robust,and low-cost titanosilicate mo-lecular sieve-based photocatalysts with industrial potential for selective oxidative transformationsand pollutant degradation.展开更多
Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes ...Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals.In this work,a facile one‐pot oil bath method has been proposed to fabricate a noble metal‐free ultrathin Ni‐doped ZnIn_(2)S_(4)(ZIS/Ni)composite nanosheet for effective solar‐driven selective dehydrocoupling of benzyl alcohol into value‐added C–C coupled hydrobenzoin and H_(2) fuel,which exhibits higher performance than pure ZIS nanosheet.The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position,which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer.Furthermore,it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products.It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.展开更多
基金supported by the Opening Project of State Key Laboratory of Advanced Chemical Power Sourcesthe Guizhou Provincial Science and Technology Projects(QKHJC-ZK[2021]YB057)+1 种基金the Growth Project of Young Scientific and Technological Talents in Colleges and Universities of Guizhou Province(QKHJCKYZ[2021]252)the Reward and Subsidy Fund Project of Guizhou Education University(Z20210108)。
文摘Two-dimensional (2D)Ni(OH)_(2) nanosheets can theoretically expose their active sites of 100%.Whereas,their intrinsic easy accumulation and low conductivity lead to weak and unsustainable reaction kinetics.Herein,we propose a novel halogen chlorine-triggered electrochemical etching strategy to controllably manage the reaction kinetics of 2D Ni(OH)_(2) nanosheets(EE/Cl-Ni(OH)_(2)).It is found that halogen chlorine doping can adjust the interlamellar spacing flexibly and promote the lattice oxygen activation to achieve controlled construction of superficial oxygen defects at the adjustable voltage.The optimal EE/Cl-Ni(OH)_(2) electrode exhibits a high rate capability and excellent specific capacity of 206.9 mA h g^(-1) at 1 A g^(-1) in a three-electrode system,which is more than twice as high as the pristine Ni(OH)_(2).Furthermore,EE/Cl-Ni(OH)_(2) cathode and FeOOH@rGO anode are employed for developing an aqueous Ni-Fe battery with an excellent energy density of 83 W h kg^(-1),a high power density of 17051 W kg^(-1),and robust durability over 20,000 cycles.This strategy exploits a fresh channel for the ingenious fabrication of highefficiency and stable nickel-based deficiency materials for energy storage.
文摘lmprovement of the charge separation of titanosilicate molecular sieves is critical to their use asphotocatalysts for oxidative organic transformations.In this work,MFI TS-1 molecular sievenanosheets(TS-1 NS)were synthesized by a low-temperature hydrothermal method using a tai-lored diquaternary ammonium surfactant as the structure-directing agent.Introducing Ni^2+cationsat the ion-exchange sites of the TS-1 NS framework significantly enhanced its photoactivity in aero-bic alcohol oxidation.The optimized Ni cation-functionalized TS-1 NS(Ni/TS-1 NS)provide impres-sive photoactivity,with a benzyl alcohol(BA)conversion of 78.9%and benzyl aldehyde(BAD)se-lectivity of 98.8%using O as the only oxidant under full light irradiation;this BAD yield is approx-imately six times greater than that obtained for bulk TS-1,and is maintained for five runs.The ex-cellent photoactivity of Ni/TS-1 NS is attributed to the significantly enlarged surface area of thetwo-dimensional morphology TS-1 NS,extra mesopores,and greatly improved charge separation.Compared with bulk TS-1,Ni/TS-1 NS has a much shorter charge transfer distance.Theas-introduced Ni species could capture the photoelectrons to further improve the charge separa-tion.This work opens the way to a class of highly selective,robust,and low-cost titanosilicate mo-lecular sieve-based photocatalysts with industrial potential for selective oxidative transformationsand pollutant degradation.
文摘Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals.In this work,a facile one‐pot oil bath method has been proposed to fabricate a noble metal‐free ultrathin Ni‐doped ZnIn_(2)S_(4)(ZIS/Ni)composite nanosheet for effective solar‐driven selective dehydrocoupling of benzyl alcohol into value‐added C–C coupled hydrobenzoin and H_(2) fuel,which exhibits higher performance than pure ZIS nanosheet.The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position,which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer.Furthermore,it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products.It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.
