The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite growth.To address these challenges,an inner Helmholtz plane(IHP)regulation method is proposed by employing low-cos...The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite growth.To address these challenges,an inner Helmholtz plane(IHP)regulation method is proposed by employing low-cost,non-toxic maltitol as the electrolyte additive.The preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane,and thus hinder the immediate contact between Zn metal and H_(2)O.Meanwhile,strong interaction between maltitol and H_(2)O molecules can restrain the activity of H_(2)O.Besides,the"IHP adsorption effect"along with the low LUMO energy level of maltitol-CF_(3)SO_(3)^(-)can promote the in-situ formation of an organic-inorganic complex solid electrolyte interface(SEI)layer.As a result,the hydrogen/oxygen evolution side reaction,corrosion,and dendrites issues are effectively suppressed,thereby leading to highly reversible and dendrite-free Zn plating/stripping.The Zn‖I_(2)battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability,showing a capacity retention of 75%over 20000 charge-discharge cycles at a large current density of 5 A g^(-1).In addition,the capacity of the device has almost no obvious decay over20000 cycles even at-30℃.This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.展开更多
The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to ...The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to form key intermediates with reactant molecules.The present study successfully synthesized a crusiform-like mesoporous structure of nitrogen-doped carbon-coated Cu_(2)O/Cu(Cu_(2)O/Cu/N-C)with a Cu_(2)O/dual electron acceptor interface using etched HKUST-1 as the precursor.A series of theoretical and experimental studies have demonstrated that the Cu_(2)O/Cu/N-C interface in the photocatalytic homo-coupling of terminal alkynes not only effectively enhances the separation of photogenerated electron−hole pairs,but also facilitates the formation of the key intermediate[Cu_(2)O/Cu/N-C]-phenylacetylide and promotes the rearrangement of its internal charges.As a result,the homo-coupling reaction can be effectively facilitated.The primary reason for the functional role of Cu_(2)O/Cu/N-C interface lies in the downward bending of energy band from Cu_(2)O to N-doped C layers,induced by the different work functions of Cu_(2)O,Cu and N-doped C layers.Consequently,Cu_(2)O/Cu/N-C photocatalysts demonstrate exceptional photocatalytic activity in the homo-coupling reaction of terminal alkynes under blue-light irradiation and air atmosphere.The present study presents a novel research methodology for the development of highly efficient visible light catalysts to facilitate organic reactions in future applications.展开更多
Recently,organic-inorganic hybrid metal halides(HMHs)have attracted extensive attention as promis-ing multifunctional materials by virtue of their structural diversity and tunable photophysical properties.However,it r...Recently,organic-inorganic hybrid metal halides(HMHs)have attracted extensive attention as promis-ing multifunctional materials by virtue of their structural diversity and tunable photophysical properties.However,it remains a challenge to design HMHs with specific functions on demand.Herein,by introduc-ing R/S-methylbenzylamine(R/S-MBA)and doping Sb^(3+),we have achieved both second harmonic gen-eration(SHG)and circularly polarized luminescence(CPL)properties in lead-free indium halides.The introduction of chiral organic cations can break the symmetry and induce the indium halides to crys-tallize in the chiral space group.The Sb^(3+)with ns2 electronic configuration can serve as the dopants to promote the formation of self-trapped excitons,so as to activate highly efficient luminescence.As a re-sult,the as-prepared Sb3+doped(R/S-MBA)3 InCl6 show not only SHG responses but also CPL signals with luminescence dissymmetry factor of−5.3×10^(−3) and 4.7×10^(−3).This work provides a new inspiration for the exploitation of chiral multifunctional materials.展开更多
TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods t...TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods to enhance the visible and near-infrared(NIR)light absorption of TiO_(2)NBs,a typical UV light photocatalyst,thus the enhancement of its full solar spectrum(UV,visible and NIR)photocatalytic antibacterial properties is achieved.Preliminary surface plasmon resonance(SPR)enhancement photocatalytic antibacterial mechanism is suggested.On one hand,transverse and longitudinal SPR of Au NRs is beneficial for visible and NIR light utilization.On the other hand,Au NRs combined with TiO_(2)NBs to form the heterostructure,which can improve the photogenerated carrier separation and direct electron transfer increases the hot electron concentration while Au NRs as the electron channel can well restrain charge recombination.finally produces the high yield of radical oxygen species and exhibits a superior antibacterial efficiency.Furthermore,we design a sterilization file cabinet with Au NR/TiO_(2)NB heterostructures as the photocatalytic coating plates.Our study reveals that Au NR/TiO_(2)NB heterostructure is a potential candidate for sterilization of bacteria and archives protection.展开更多
基金supported by the National Natural Science Foundation of China(52261160384)the Shenzhen Science and Technology Innovation Commission(RCYX20221008092934093)+1 种基金the Shenzhen Science and Technology Program(KJZD20230923114107014)the support from Testing Technology Center of Materials and Devices,Tsinghua Shenzhen International Graduate School。
文摘The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite growth.To address these challenges,an inner Helmholtz plane(IHP)regulation method is proposed by employing low-cost,non-toxic maltitol as the electrolyte additive.The preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane,and thus hinder the immediate contact between Zn metal and H_(2)O.Meanwhile,strong interaction between maltitol and H_(2)O molecules can restrain the activity of H_(2)O.Besides,the"IHP adsorption effect"along with the low LUMO energy level of maltitol-CF_(3)SO_(3)^(-)can promote the in-situ formation of an organic-inorganic complex solid electrolyte interface(SEI)layer.As a result,the hydrogen/oxygen evolution side reaction,corrosion,and dendrites issues are effectively suppressed,thereby leading to highly reversible and dendrite-free Zn plating/stripping.The Zn‖I_(2)battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability,showing a capacity retention of 75%over 20000 charge-discharge cycles at a large current density of 5 A g^(-1).In addition,the capacity of the device has almost no obvious decay over20000 cycles even at-30℃.This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.
基金supported by the Xuzhou Key Research and Development Program(Social Development)(No.KC23298)the National Natural Science Foundation of China(No.22271122)+1 种基金the Natural Science Foundation of Jiangsu Province(No.BK20211549)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_2903).
文摘The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to form key intermediates with reactant molecules.The present study successfully synthesized a crusiform-like mesoporous structure of nitrogen-doped carbon-coated Cu_(2)O/Cu(Cu_(2)O/Cu/N-C)with a Cu_(2)O/dual electron acceptor interface using etched HKUST-1 as the precursor.A series of theoretical and experimental studies have demonstrated that the Cu_(2)O/Cu/N-C interface in the photocatalytic homo-coupling of terminal alkynes not only effectively enhances the separation of photogenerated electron−hole pairs,but also facilitates the formation of the key intermediate[Cu_(2)O/Cu/N-C]-phenylacetylide and promotes the rearrangement of its internal charges.As a result,the homo-coupling reaction can be effectively facilitated.The primary reason for the functional role of Cu_(2)O/Cu/N-C interface lies in the downward bending of energy band from Cu_(2)O to N-doped C layers,induced by the different work functions of Cu_(2)O,Cu and N-doped C layers.Consequently,Cu_(2)O/Cu/N-C photocatalysts demonstrate exceptional photocatalytic activity in the homo-coupling reaction of terminal alkynes under blue-light irradiation and air atmosphere.The present study presents a novel research methodology for the development of highly efficient visible light catalysts to facilitate organic reactions in future applications.
基金supported by the National Funds for Distinguished Young Scientists(No.61825503)the National Natural Science Foundation of China(Nos.62288102,62375142,22161160318).
文摘Recently,organic-inorganic hybrid metal halides(HMHs)have attracted extensive attention as promis-ing multifunctional materials by virtue of their structural diversity and tunable photophysical properties.However,it remains a challenge to design HMHs with specific functions on demand.Herein,by introduc-ing R/S-methylbenzylamine(R/S-MBA)and doping Sb^(3+),we have achieved both second harmonic gen-eration(SHG)and circularly polarized luminescence(CPL)properties in lead-free indium halides.The introduction of chiral organic cations can break the symmetry and induce the indium halides to crys-tallize in the chiral space group.The Sb^(3+)with ns2 electronic configuration can serve as the dopants to promote the formation of self-trapped excitons,so as to activate highly efficient luminescence.As a re-sult,the as-prepared Sb3+doped(R/S-MBA)3 InCl6 show not only SHG responses but also CPL signals with luminescence dissymmetry factor of−5.3×10^(−3) and 4.7×10^(−3).This work provides a new inspiration for the exploitation of chiral multifunctional materials.
基金fundings from the National Natural Science Foundation of China(Nos.51872173,51772176)TaishanScholars Program of Shandong Province(Nos.tsqn201812068,tspd20161006)+6 种基金Higher School Youth Innovation Team of Shandong Province(No.2019KJA013)Key Research and Development Program of Shandong Province(No.2018GGX102028)Science and Technology Special Project of Qingdao City(No.20-3-4-3-nsh)the Opening Fund of State Key Laboratory of Heavy Oil Processing(No.SKLOP202002006)Cooperative Education Project of the Ministry of Education(No.201902195026)Humanities and Social Sciences Program(GoMoruo Studies)of the Education Department of Sichuan Province(No.GY2020C01)Shandong Archives Science and Technology Project(No.2020-33)。
文摘TiO_(2)photocatalysts have been widely studied and applied for removing bacteria,but its antibacterial efficiency is limited to the ultraviolet(UV)range of the solar spectrum.In this work,we use the gold(Au)nanorods to enhance the visible and near-infrared(NIR)light absorption of TiO_(2)NBs,a typical UV light photocatalyst,thus the enhancement of its full solar spectrum(UV,visible and NIR)photocatalytic antibacterial properties is achieved.Preliminary surface plasmon resonance(SPR)enhancement photocatalytic antibacterial mechanism is suggested.On one hand,transverse and longitudinal SPR of Au NRs is beneficial for visible and NIR light utilization.On the other hand,Au NRs combined with TiO_(2)NBs to form the heterostructure,which can improve the photogenerated carrier separation and direct electron transfer increases the hot electron concentration while Au NRs as the electron channel can well restrain charge recombination.finally produces the high yield of radical oxygen species and exhibits a superior antibacterial efficiency.Furthermore,we design a sterilization file cabinet with Au NR/TiO_(2)NB heterostructures as the photocatalytic coating plates.Our study reveals that Au NR/TiO_(2)NB heterostructure is a potential candidate for sterilization of bacteria and archives protection.
