Silicon (Si) is a promising anode material for next-generation high-energy lithium-ion batteries (LIBs) due to its high capacity.However,the large volumetric expansion,poor ion conductivity and unstable solid electrol...Silicon (Si) is a promising anode material for next-generation high-energy lithium-ion batteries (LIBs) due to its high capacity.However,the large volumetric expansion,poor ion conductivity and unstable solid electrolyte interface (SEI) lead to rapid capacity fading and low rate performance.Herein,we report Si nitride (SiN) comprising stoichiometric Si_(3)N_(4) and Li-active anazotic SiN_(x) coated porous Si (p-Si@SiN)for high-performance anodes in LIBs.The ant-nest-like porous Si consisting of 3D interconnected Si nanoligaments and bicontinuous nanopores prevents pulverization and accommodates volume expansion during cycling.The Si_(3)N_(4) offers mechanically protective coating to endow highly structural integrity and inhibit superfluous formation of SEI.The fast ion conducting Li_(3)N generated in situ from lithiation of active SiN_(x) facilitates Li ion transport.Consequently,the p-Si@SiN anode has appealing electrochemical properties such as a high capacity of 2180 mAh g^(-1)at 0.5 A g^(-1) with 84%capacity retention after 200cycles and excellent rate capacity with discharge capacity of 721 mAh g^(-1) after 500 cycles at 5.0 A g^(-1).This work provides insights into the rational design of active/inactive nanocoating on Si-based anode materials for fast-charging and highly stable LIBs.展开更多
The co-precipitation derived LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 cathode material was modified by a coating layer of TiP_2O_7 through an ethanol-based process. The TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 is charac...The co-precipitation derived LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 cathode material was modified by a coating layer of TiP_2O_7 through an ethanol-based process. The TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 is characterized by Xray diffraction analysis, scanning electron microscopy and transmission electron microscopy to investigate the microstructure and morphology. The differential scanning calorimetry was employed to confirm the improved thermal stability. The electrochemical properties were evaluated by the constant-current charge/discharge tests. The TiP_2O_7 coating layer is effectively suppressing the structural degradation and ameliorating the surface status of LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 particles, and the intrinsic rhombohedral layered structure of TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 was well maintained during the long-term cycling process, while the surface structure of pristine LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 was degraded from rhombohedral R3 m layered structure to cubic rock-salt structure. The charged state Ni^(4+) ions will easily transform into Ni^(2+) when the electrolytes oxidized at the interface of cathode/electrolytes and formed the cubic rock-salt NiO type structure, and the cubic rock-salt structure without electrochemical activity on the surface of LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 particles will finally accelerate capacity fading. The thermal stability and cyclic performances of the LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 electrode were remarkably improved by TiP_2O_7 coating, the total amount of heat release corresponding to the intensity of thermal runaway were 1075.5 and 964.6 J/g for pristine LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 and TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 respectively, the pouch shaped full cells that employed TiP 2 O7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 as cathode were able to perform more than 2200 cycles at 25 ℃ and more than 1000 cycles at 45 ℃ before the capacity retention fading to 80%.展开更多
There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to i...There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.展开更多
The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migr...The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migration.Herein,we prepare a dual-salt poly(tetrahydrofuran)-based electrolyte consisting of lithium hexafluorophosphate and lithium difluoro(oxalato)borate(LiDFOB).The Li-salt anions(DFOB−)not only accelerate the ring-opening polymerization of tetrahydrofuran,but also promote the formation of highly ion-conductive and sustainable interphases on Li metal anodes without sacrificing the Li^(+)conductivity of electrolytes,which is favorable for Li^(+)transport kinetics at low temperatures.Applications of this polymer electrolyte in Li||LiFePO_(4)cells show 82.3%capacity retention over 1000 cycles at 30℃and endow stable discharge capacity at−30℃.Remarkably,the Li||LiFePO4 cells retain 52%of their room-temperature capacity at−20℃and 0.1 C.This rational design of dual-salt polymer-based electrolytes may provide a new perspective for the stable operation of quasi-solid-state batteries at low temperatures.展开更多
Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous io...Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.展开更多
Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can impr...Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.展开更多
Large-scale deployment of Internet of Things (IoT),a revolutionary innovation for a better world,is hampered by the limitation of energy self-sufficiency.Constructing transition metal nitride (TMN)-based micro-superca...Large-scale deployment of Internet of Things (IoT),a revolutionary innovation for a better world,is hampered by the limitation of energy self-sufficiency.Constructing transition metal nitride (TMN)-based micro-supercapacitors is a possible solution by taking advantage of the high conductivity,large specific capacitance,and large tap density of the materials.However,the pseudocapacitive storage mechanism of TMNs is still unclear consequently impeding the design of microdevices.Herein,the functions and mechanism of TMNs with different metal oxynitride (TMNO_(x)) concentrations in pseudocapacitive electrodes are investigated systematically by in situ Raman scattering,ex situ X-ray photoelectron spectroscopy,as well as ion isolation and substitution cyclic voltammetry.It is found that the specific capacitances of TMNs depend on the TMNO_(x) concentrations and the N–M–O site is responsible for the large pseudocapacitance via the Faradic reaction between TMNO_(x) and OH^(-).Our study elucidates the mechanism pertaining to pseudocapacitive charge storage of TMNs and provides insights into the design and optimization of TMNO_(x) as well as other electrode materials for pseudocapacitors.展开更多
In the scope of developing new electrochemical concepts to build batteries with high energy density,chloride ion batteries(CIBs)have emerged as a candidate for the next generation of novel electrochemical energy stora...In the scope of developing new electrochemical concepts to build batteries with high energy density,chloride ion batteries(CIBs)have emerged as a candidate for the next generation of novel electrochemical energy storage technologies,which show the potential in matching or even surpassing the current lithium metal batteries in terms of energy density,dendrite-free safety,and elimination of the dependence on the strained lithium and cobalt resources.However,the development of CIBs is still at the initial stage with unsatisfactory performance and several challenges have hindered them from reaching commercialization.In this review,we examine the current advances of CIBs by considering the electrode material design to the electrolyte,thus outlining the new opportunities of aqueous CIBs especially combined with desalination,chloride redox battery,etc.With respect to the developing road of lithium ion and fluoride ion batteries,the possibility of using solid-state chloride ion conductors to replace liquid electrolytes is tentatively discussed.Going beyond,perspectives and clear suggestions are concluded by highlighting the major obstacles and by prescribing specific research topics to inspire more efforts for CIBs in large-scale energy storage applications.展开更多
Several challenging issues,such as the poor conductivity of sulfur,shuttle effects,large volume change of cathode,and the dendritic lithium in anode,have led to the low utilization of sulfur and hampered the commercia...Several challenging issues,such as the poor conductivity of sulfur,shuttle effects,large volume change of cathode,and the dendritic lithium in anode,have led to the low utilization of sulfur and hampered the commercialization of lithium–sulfur batteries.In this study,a novel three-dimensionally interconnected network structure comprising Co9 S8 and multiwalled carbon nanotubes(MWCNTs)was synthesized by a solvothermal route and used as the sulfur host.The assembled batteries delivered a specific capacity of1154 m Ah g-1 at 0.1 C,and the retention was 64%after 400 cycles at 0.5 C.The polar and catalytic Co9 S8 nanoparticles have a strong adsorbent effect for polysulfide,which can effectively reduce the shuttling effect.Meanwhile,the three-dimensionally interconnected CNT networks improve the overall conductivity and increase the contact with the electrolyte,thus enhancing the transport of electrons and Li ions.Polysulfide adsorption is greatly increased with the synergistic effect of polar Co9 S8 and MWCNTs in the three-dimensionally interconnected composites,which contributes to their promising performance for the lithium–sulfur batteries.展开更多
Lithium sulfur battery(LSB)is a promising energy storage system to meet the increasing energy demands for electric vehicles and smart grid,while its wide commercialization is severely inhibited by the"shuttle eff...Lithium sulfur battery(LSB)is a promising energy storage system to meet the increasing energy demands for electric vehicles and smart grid,while its wide commercialization is severely inhibited by the"shuttle effect"of polysulfides,low utilization of sulfur cathode,and safety of lithium anode.To overcome these issues,herein,monodisperse polar NiCo_(2)O_(4)nanoparticles decorated porous graphene aerogel composite(NCO-GA)is proposed.The aerogel composite demonstrates high conductivity,hierarchical porous structure,high chemisorption capacity and excellent electrocatalytic ability,which effectively inhibits the"shuttle effect",promotes the ion/electron transport and increases the reaction kinetics.The NCO-GA/S cathode exhibits high discharge specific capacity(1214.1 mAh g^(-1)at 0.1 C),outstanding rate capability(435.7 mAh g^(-1)at 5 C)and remarkable cycle stability(decay of 0.031%/cycle over 1000 cycles).Quantitative analyses show that the physical adsorption provided by GA mainly contributes to the capacity of NCO-GA/S at low rate,while the chemical adsorption provided by polar NiCo_(2)O_(4)contributes mainly to the capacity of NCO-GA/S with the increase of current density and cycling.This work provides a new strategy for the design of GA-based composite with synergistic adsorption and electrocatalytic activity for the potential applications in LSB and related energy fields.展开更多
基金financially supported by the National Natural Science Foundation of China (U2004210, 51974208, U2003130, 21875080, 52002297)the Outstanding Youth Foundation of Natural Science Foundation of Hubei Province (2020CFA099)+2 种基金the Special Project of Central Government for Local Science and Technology Development of Hubei Province (2019ZYYD024)the Innovation group of Natural Science Foundation of Hubei Province (2019CFA020)the City University of Hong Kong Strategic Research Grants (7005505)。
文摘Silicon (Si) is a promising anode material for next-generation high-energy lithium-ion batteries (LIBs) due to its high capacity.However,the large volumetric expansion,poor ion conductivity and unstable solid electrolyte interface (SEI) lead to rapid capacity fading and low rate performance.Herein,we report Si nitride (SiN) comprising stoichiometric Si_(3)N_(4) and Li-active anazotic SiN_(x) coated porous Si (p-Si@SiN)for high-performance anodes in LIBs.The ant-nest-like porous Si consisting of 3D interconnected Si nanoligaments and bicontinuous nanopores prevents pulverization and accommodates volume expansion during cycling.The Si_(3)N_(4) offers mechanically protective coating to endow highly structural integrity and inhibit superfluous formation of SEI.The fast ion conducting Li_(3)N generated in situ from lithiation of active SiN_(x) facilitates Li ion transport.Consequently,the p-Si@SiN anode has appealing electrochemical properties such as a high capacity of 2180 mAh g^(-1)at 0.5 A g^(-1) with 84%capacity retention after 200cycles and excellent rate capacity with discharge capacity of 721 mAh g^(-1) after 500 cycles at 5.0 A g^(-1).This work provides insights into the rational design of active/inactive nanocoating on Si-based anode materials for fast-charging and highly stable LIBs.
基金supported by the National Natural Science Foundation of China (No. 51372178)the Natural Science Foundation for Distinguished Young Scholars of Hubei Province of China (No. 2013CFA021)
文摘The co-precipitation derived LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 cathode material was modified by a coating layer of TiP_2O_7 through an ethanol-based process. The TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 is characterized by Xray diffraction analysis, scanning electron microscopy and transmission electron microscopy to investigate the microstructure and morphology. The differential scanning calorimetry was employed to confirm the improved thermal stability. The electrochemical properties were evaluated by the constant-current charge/discharge tests. The TiP_2O_7 coating layer is effectively suppressing the structural degradation and ameliorating the surface status of LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 particles, and the intrinsic rhombohedral layered structure of TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 was well maintained during the long-term cycling process, while the surface structure of pristine LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 was degraded from rhombohedral R3 m layered structure to cubic rock-salt structure. The charged state Ni^(4+) ions will easily transform into Ni^(2+) when the electrolytes oxidized at the interface of cathode/electrolytes and formed the cubic rock-salt NiO type structure, and the cubic rock-salt structure without electrochemical activity on the surface of LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 particles will finally accelerate capacity fading. The thermal stability and cyclic performances of the LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 electrode were remarkably improved by TiP_2O_7 coating, the total amount of heat release corresponding to the intensity of thermal runaway were 1075.5 and 964.6 J/g for pristine LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 and TiP_2O_7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 respectively, the pouch shaped full cells that employed TiP 2 O7-coated LiNi_(0.8)Co_(0.15)Al_(0.05)O_2 as cathode were able to perform more than 2200 cycles at 25 ℃ and more than 1000 cycles at 45 ℃ before the capacity retention fading to 80%.
基金financially supported by the 2022 Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(STKJ202209077 and STKJ202209083)the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2019(GDUPS2019)the City University of Hong Kong Strategic Research Grant(SRG)(7005505)。
文摘There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.
基金funding from the Natural Science Foundation of Hubei Province,China(Grant No.2022CFA031)supported by the Natural Science Foundation of China(Grant No.22309056).
文摘The stable operation of solid-state lithium metal batteries at low temperatures is plagued by severe restrictions from inferior electrolyte-electrode interface compatibility and increased energy barrier for Li^(+)migration.Herein,we prepare a dual-salt poly(tetrahydrofuran)-based electrolyte consisting of lithium hexafluorophosphate and lithium difluoro(oxalato)borate(LiDFOB).The Li-salt anions(DFOB−)not only accelerate the ring-opening polymerization of tetrahydrofuran,but also promote the formation of highly ion-conductive and sustainable interphases on Li metal anodes without sacrificing the Li^(+)conductivity of electrolytes,which is favorable for Li^(+)transport kinetics at low temperatures.Applications of this polymer electrolyte in Li||LiFePO_(4)cells show 82.3%capacity retention over 1000 cycles at 30℃and endow stable discharge capacity at−30℃.Remarkably,the Li||LiFePO4 cells retain 52%of their room-temperature capacity at−20℃and 0.1 C.This rational design of dual-salt polymer-based electrolytes may provide a new perspective for the stable operation of quasi-solid-state batteries at low temperatures.
基金support from the National Natural Science Foundation of China(32171728)Wuhan Knowledge Innovation Project(2022020801020312).
文摘Thick electrodes can reduce the ratio of inactive constituents in a holistic energy storage system while improving energy and power densities.Unfortunately,traditional slurry-casting electrodes induce high-tortuous ionic diffusion routes that directly depress the capacitance with a thickening design.To overcome this,a novel 3D low-tortuosity,self-supporting,wood-structured ultrathick electrode(NiMoN@WC,a thickness of~1400 mm)with hierarchical porosity and artificial array-distributed small holes was constructed via anchoring bimetallic nitrides into the monolithic wood carbons.Accompanying the embedded NiMoN nanoclusters with well-designed geometric and electronic structure,the vertically low-tortuous channels,enlarged specific surface area and pore volume,superhydrophilic interface,and excellent charge conductivities,a superior capacitance of NiMoN@WC thick electrodes(~5350 mF cm^(-2)and 184.5 F g^(-1))is achieved without the structural deformation.In especial,monolithic wood carbons with gradient porous network not only function as the high-flux matrices to ameliorate the NiMoN loading via cell wall engineering but also allow fully-exposed electroactive substance and efficient current collection,thereby deliver an acceptable rate capability over 75%retention even at a high sweep rate of 20 mA cm^(-2).Additionally,an asymmetric NiMoN@WC//WC supercapacitor with an available working voltage of 1.0-1.8 V is assembled to demonstrate a maximum energy density of~2.04 mWh cm^(-2)(17.4 Wh kg^(-1))at a power density of 1620 mW cm^(-2),along with a decent long-term lifespan over 10,000 charging-discharging cycles.As a guideline,the rational design of wood ultrathick electrode with nanostructured transition metal nitrides sketch a promising blueprint for alleviating global energy scarcity while expanding carbon-neutral technologies.
基金financially supported by the Key Research and Development Program of Hubei Province (2021BAA208)the National Natural Science Foundation of China (52002294,51974208 and U2003130)+3 种基金the Young Top-notch Talent Cultivation Program of Hubei ProvinceKnowledge Innovation Program of Wuhan-Shuguang Project (2022010801020364)the City University of Hong Kong Strategic Research Grant (SRG) (7005505)the City University of Hong Kong Donation Research Grant (DONRMG 9229021)。
文摘Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.
基金financially supported by the Hong Kong Scholars Program (XJ2018009)the City University of Hong Kong Strategic Research Grant (SRG) (7005505)+3 种基金the Shenzhen – Hong Kong Innovative Collaborative Research and Development Program (SGLH20181109110802117 and CityU 9240014)the National Natural Science Foundation of China(U2004210, 21875080, 51572100 and 52003129)the Innovative Research Group Project of the Natural Science Foundation of Hubei Province (2019CFA020)the Shandong Provincial Natural Science Foundation (ZR2019BB006)。
文摘Large-scale deployment of Internet of Things (IoT),a revolutionary innovation for a better world,is hampered by the limitation of energy self-sufficiency.Constructing transition metal nitride (TMN)-based micro-supercapacitors is a possible solution by taking advantage of the high conductivity,large specific capacitance,and large tap density of the materials.However,the pseudocapacitive storage mechanism of TMNs is still unclear consequently impeding the design of microdevices.Herein,the functions and mechanism of TMNs with different metal oxynitride (TMNO_(x)) concentrations in pseudocapacitive electrodes are investigated systematically by in situ Raman scattering,ex situ X-ray photoelectron spectroscopy,as well as ion isolation and substitution cyclic voltammetry.It is found that the specific capacitances of TMNs depend on the TMNO_(x) concentrations and the N–M–O site is responsible for the large pseudocapacitance via the Faradic reaction between TMNO_(x) and OH^(-).Our study elucidates the mechanism pertaining to pseudocapacitive charge storage of TMNs and provides insights into the design and optimization of TMNO_(x) as well as other electrode materials for pseudocapacitors.
基金the support of the National Energy-Saving and Low-Carbon Materials Production and Application Demonstration Platform Program (TC220H06N)the National Natural Science Foundation of China (51832004,51972259,52127816)the Natural Science Foundation of Hubei Province (2022CFA087)。
文摘In the scope of developing new electrochemical concepts to build batteries with high energy density,chloride ion batteries(CIBs)have emerged as a candidate for the next generation of novel electrochemical energy storage technologies,which show the potential in matching or even surpassing the current lithium metal batteries in terms of energy density,dendrite-free safety,and elimination of the dependence on the strained lithium and cobalt resources.However,the development of CIBs is still at the initial stage with unsatisfactory performance and several challenges have hindered them from reaching commercialization.In this review,we examine the current advances of CIBs by considering the electrode material design to the electrolyte,thus outlining the new opportunities of aqueous CIBs especially combined with desalination,chloride redox battery,etc.With respect to the developing road of lithium ion and fluoride ion batteries,the possibility of using solid-state chloride ion conductors to replace liquid electrolytes is tentatively discussed.Going beyond,perspectives and clear suggestions are concluded by highlighting the major obstacles and by prescribing specific research topics to inspire more efforts for CIBs in large-scale energy storage applications.
基金National Natural Science Foundation of China(No.51974209)the Natural Science Foundation of Hubei Province of China(Nos.2013CFA021,2017CFB401,2018CFA022)。
文摘Several challenging issues,such as the poor conductivity of sulfur,shuttle effects,large volume change of cathode,and the dendritic lithium in anode,have led to the low utilization of sulfur and hampered the commercialization of lithium–sulfur batteries.In this study,a novel three-dimensionally interconnected network structure comprising Co9 S8 and multiwalled carbon nanotubes(MWCNTs)was synthesized by a solvothermal route and used as the sulfur host.The assembled batteries delivered a specific capacity of1154 m Ah g-1 at 0.1 C,and the retention was 64%after 400 cycles at 0.5 C.The polar and catalytic Co9 S8 nanoparticles have a strong adsorbent effect for polysulfide,which can effectively reduce the shuttling effect.Meanwhile,the three-dimensionally interconnected CNT networks improve the overall conductivity and increase the contact with the electrolyte,thus enhancing the transport of electrons and Li ions.Polysulfide adsorption is greatly increased with the synergistic effect of polar Co9 S8 and MWCNTs in the three-dimensionally interconnected composites,which contributes to their promising performance for the lithium–sulfur batteries.
基金supported by the National Natural Science Foundation of China(51974209)the Outstanding Doctoral Award Fund in Shanxi Province(20202017)。
文摘Lithium sulfur battery(LSB)is a promising energy storage system to meet the increasing energy demands for electric vehicles and smart grid,while its wide commercialization is severely inhibited by the"shuttle effect"of polysulfides,low utilization of sulfur cathode,and safety of lithium anode.To overcome these issues,herein,monodisperse polar NiCo_(2)O_(4)nanoparticles decorated porous graphene aerogel composite(NCO-GA)is proposed.The aerogel composite demonstrates high conductivity,hierarchical porous structure,high chemisorption capacity and excellent electrocatalytic ability,which effectively inhibits the"shuttle effect",promotes the ion/electron transport and increases the reaction kinetics.The NCO-GA/S cathode exhibits high discharge specific capacity(1214.1 mAh g^(-1)at 0.1 C),outstanding rate capability(435.7 mAh g^(-1)at 5 C)and remarkable cycle stability(decay of 0.031%/cycle over 1000 cycles).Quantitative analyses show that the physical adsorption provided by GA mainly contributes to the capacity of NCO-GA/S at low rate,while the chemical adsorption provided by polar NiCo_(2)O_(4)contributes mainly to the capacity of NCO-GA/S with the increase of current density and cycling.This work provides a new strategy for the design of GA-based composite with synergistic adsorption and electrocatalytic activity for the potential applications in LSB and related energy fields.
