Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish...Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.展开更多
Lithium–sulfur(Li-S)batteries have the advantages of high theoretical specific capacity(1675 mAh g^(−1)),rich sulfur resources,low production cost,and friendly environment,which makes it one of the most promising nex...Lithium–sulfur(Li-S)batteries have the advantages of high theoretical specific capacity(1675 mAh g^(−1)),rich sulfur resources,low production cost,and friendly environment,which makes it one of the most promising next-generation rechargeable energy storage devices.However,the“shuttle effect”of polysulfide results in the passivation of metal lithium anode,the decrease of battery capacity and coulombic efficiency,and the deterioration of cycle stability.To realize the commercialization of Li-S batteries,its serious“shuttle effect”needs to be suppress.The commercial separators are ineffective to suppress this effect because of its large pore size.Therefore,it is an effective strategy to modify the separator surface and introduce functional modified layer.In addition to the blocking strategy,the catalysis of polysulfide conversion reaction is also an important factor hindering the migration of polysulfides.In this review,the principles of separator modification,functionalization,and catalysis in Li-S batteries are reviewed.Furthermore,the research trend of separator functionalization and polysulfide catalysis in the future is prospected.展开更多
Using porous carbon hosts in cathodes of Li-S cells can disperse S actives and offset their poor electrical conductivity.However,such reservoirs would in turn absorb excess electrolyte solvents to S-unfilled regions,c...Using porous carbon hosts in cathodes of Li-S cells can disperse S actives and offset their poor electrical conductivity.However,such reservoirs would in turn absorb excess electrolyte solvents to S-unfilled regions,causing the electrolyte overconsumption,specific energy decline,and even safety hazards for battery devices.To build better cathodes,we propose to substitute carbons by In-doped SnO_(2)(ITO)nano ceramics that own three-in-one functionalities:1)using conductive ITO enables minimizing the total carbon content to an extremely low mass ratio(~3%)in cathodes,elevating the electrode tap density and averting the electrolyte overuse;2)polar ITO nanoclusters can serve as robust anchors toward Li polysulfide(LiPS)by electrostatic adsorption or chemical bond interactions;3)they offer catalysis centers for liquid–solid phase conversions of S-based actives.Also,such ceramics are intrinsically nonflammable,preventing S cathodes away from thermal runaway or explosion.These merits entail our configured cathodes with high tap density(1.54 g cm^(−3)),less electrolyte usage,good security for flame retardance,and decent Li-storage behaviors.With lean and LiNO_(3)-free electrolyte,packed full cells exhibit excellent redox kinetics,suppressed LiPS shuttling,and excellent cyclability.This may trigger great research enthusiasm in rational design of low-carbon and safer S cathodes.展开更多
Sulfur and selenium have been paid more and more attention in energy storage systems because of their high theoretical specific gravimetric and volumetric capacities.With the increasing scarcity of lithium resources,s...Sulfur and selenium have been paid more and more attention in energy storage systems because of their high theoretical specific gravimetric and volumetric capacities.With the increasing scarcity of lithium resources,secondary batteries made of sulfur and selenium coupled with other alkali metal/alkaline earth metals(e.g.Na,K,Mg)are expected to play a vital role in future production and human life.Due to the volume expansion,poor conductivity and shuttle effect,the structure design of cathode,as one of the important roles in metal-S/Se batteries,has always been a hot and difficult point.In the review,various host materials of S and Se are clarified and discussed.Typically,carbonaceous materials are the most widely used hosts,while polar materials are becoming more and more popular in metal-S/Se batteries.Through a comprehensive overview,it is hoped that previous research experiences can provide further reference and guidance for the sustainable development of metal-S/Se batteries.展开更多
With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide at...With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide attention as a bridge between sustainable energy sources and daily life.展开更多
Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of po...Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of polysulfides dissolution/shuttling and poor electrical conductivity for S-based cathodes.However,extensive use of conductive carbon fillers in cell designs/technology would induce electrolytic overconsumption and thereby shelve high-energy-density promise of Li-S cells.To cut down carbon usage,we propose the incorporation of multi-functionalized NiFe2O4 quantum dots(QDs) as affordable additive substitutes.The total carbon content can be greatly curtailed from 26%(in traditional S/C cathodes) to a low/commercial mass ratio(~5%).Particularly,note that NiFe2O4 QDs additives own superb chemisorption interactions with soluble Li2Sn molecules and proper catalytic features facilitating polysulfide phase conversions and can also strengthen charge-transfer capability/redox kinetics of overall cathode systems.Benefiting from these intrinsic properties,such hybrid cathodes demonstrate prominent rate behaviors(decent capacity retention with ~526 mAh g^-1 even at 5 A g^-1) and stable cyclic performance in LiNO3-free electrolytes(only ~0.08% capacity decay per cycle in 500 cycles at 0.2 A g^-1).This work may arouse tremendous research interest in seeking other alternative QDs and offer an economical/more applicable methodology to construct low-carbon-content electrodes for practical usage.展开更多
Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”bio...Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”biomimetic design proposed for high performance Na–S batteries,where the leaves constructed from Co nanoparticles on carbon nanofibers(CNF)are fully to expose the active sites of Co.The CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the Co leaves.As an effective electrocatalytic battery system,the 3D“branch-leaf”conductive network with abundant active sites and voids can effectively trap polysulfides and provide plentiful electron/ions pathways for electrochemical reaction.DFT calculation reveals that the Co nanoparticles can induce the formation of a unique Co–S–Na molecular layer on the Co surface,which can enable a fast reduction reaction of the polysulfides.Therefore,the prepared“branch-leaf”CNF-L@Co/S electrode exhibits a high initial specific capacity of 1201 mAh g^−1 at 0.1 C and superior rate performance.展开更多
Although research interest in aqueous metal-sulfur batteries(AMSs)has surged due to their intrinsic low cost and high capacity,the practical application of AMSs remains a considerable challenge because of the restrict...Although research interest in aqueous metal-sulfur batteries(AMSs)has surged due to their intrinsic low cost and high capacity,the practical application of AMSs remains a considerable challenge because of the restrictive cycling stability.To circumvent this issue,we propose an innovative and simple pre-copper strategy to realize a high-durability aqueous Cu-S battery.The precopper strategy can effectively promote a stable metal dissolution/deposition,compensate for charge carriers,and facilitate reaction kinetics during the subsequent process.As a result,the aqueous Cu-S battery when coupled with S-decorated porous Ti_(3)C_(2)(S-d-Ti_(3)C_(2))exhibits excellent electrochemical performance,delivering a highly reversible capacity of 1805.4 mAh·g^(-1)in the initial cycle at 0.8 A·g^(-1),impressive cycling stability with 90.2%capacity retention over 800 cycles,and ultralow polarization~0.08 V even at a high current density of 3.1 A·g^(-1).The findings obtained in this work could pave the way for the design of highperformance sulfur-based aqueous batteries,which fill the vacancy of the necessary metal anode,delivering merits in both cost and cycle life.展开更多
Electrocatalytic water splitting offers a sustainable route for hydrogen production,enabling the clean and renewable alternative energy system of hydrogen economy.The scarcity and high-cost of platinum-group-metal(PGM...Electrocatalytic water splitting offers a sustainable route for hydrogen production,enabling the clean and renewable alternative energy system of hydrogen economy.The scarcity and high-cost of platinum-group-metal(PGM)materials urge the exploration of high-performance non-PGM electrocatalysts.Herein,a unique hierarchical structure of NiA/2O3 with extraordinary electrocatalytic performance(e.g.t overpotentials as low as 22 mV at 20 mA·cm^-2 and 94 mV at 100 mA·cm^-2)toward hydrogen evolution reaction in alkaline electrolyte(1 M KOH)is reported.The investigation on the hierarchical NiA/2O3 with a bimodal size-distribution also offers insight of interfacial engineering that only proper NiA/2O3 interface can effectively improve H20 adsorption,H20 dissociation as well as H adsorption,for an efficient hydrogen production.展开更多
基金financially supported by National Natural Science Foundation of China (22209133, 22272131, 21972111, 22211540712)Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX1411)+1 种基金Chongqing Engineering Research Center for Micro-Nano Biomedical Materials and DevicesChongqing Key Laboratory for Advanced Materials and Technologies。
文摘Electrolytic aqueous zinc-manganese(Zn–Mn) batteries have the advantage of high discharge voltage and high capacity due to two-electron reactions. However, the pitfall of electrolytic Zn–Mn batteries is the sluggish deposition reaction kinetics of manganese oxide during the charge process and short cycle life. We show that, incorporating ZnO electrolyte additive can form a neutral and highly viscous gel-like electrolyte and render a new form of electrolytic Zn–Mn batteries with significantly improved charging capabilities. Specifically, the ZnO gel-like electrolyte activates the zinc sulfate hydroxide hydrate assisted Mn^(2+) deposition reaction and induces phase and structure change of the deposited manganese oxide(Zn_(2)Mn_(3)O_8·H_(2)O nanorods array), resulting in a significant enhancement of the charge capability and discharge efficiency. The charge capacity increases to 2.5 mAh cm^(-2) after 1 h constant-voltage charging at 2.0 V vs. Zn/Zn^(2+), and the capacity can retain for up to 2000 cycles with negligible attenuation. This research lays the foundation for the advancement of electrolytic Zn–Mn batteries with enhanced charging capability.
基金support of the National Natural Science Foundation of China(No.21773188,No.22179109)central universities fundamental research fund(XDJK2019AA002)Chongqing Natural Science fund(cstc2020jcyj-bshx0047,cstc2021jcyj-bsh0173).
文摘Lithium–sulfur(Li-S)batteries have the advantages of high theoretical specific capacity(1675 mAh g^(−1)),rich sulfur resources,low production cost,and friendly environment,which makes it one of the most promising next-generation rechargeable energy storage devices.However,the“shuttle effect”of polysulfide results in the passivation of metal lithium anode,the decrease of battery capacity and coulombic efficiency,and the deterioration of cycle stability.To realize the commercialization of Li-S batteries,its serious“shuttle effect”needs to be suppress.The commercial separators are ineffective to suppress this effect because of its large pore size.Therefore,it is an effective strategy to modify the separator surface and introduce functional modified layer.In addition to the blocking strategy,the catalysis of polysulfide conversion reaction is also an important factor hindering the migration of polysulfides.In this review,the principles of separator modification,functionalization,and catalysis in Li-S batteries are reviewed.Furthermore,the research trend of separator functionalization and polysulfide catalysis in the future is prospected.
基金support by the National Natural Science Foundation of China(51802269,21773138)Fundamental Research Funds for the Central Universities(XDJK2019AA002)+1 种基金the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2018027)the innovation platform for academicians of Hainan province.
文摘Using porous carbon hosts in cathodes of Li-S cells can disperse S actives and offset their poor electrical conductivity.However,such reservoirs would in turn absorb excess electrolyte solvents to S-unfilled regions,causing the electrolyte overconsumption,specific energy decline,and even safety hazards for battery devices.To build better cathodes,we propose to substitute carbons by In-doped SnO_(2)(ITO)nano ceramics that own three-in-one functionalities:1)using conductive ITO enables minimizing the total carbon content to an extremely low mass ratio(~3%)in cathodes,elevating the electrode tap density and averting the electrolyte overuse;2)polar ITO nanoclusters can serve as robust anchors toward Li polysulfide(LiPS)by electrostatic adsorption or chemical bond interactions;3)they offer catalysis centers for liquid–solid phase conversions of S-based actives.Also,such ceramics are intrinsically nonflammable,preventing S cathodes away from thermal runaway or explosion.These merits entail our configured cathodes with high tap density(1.54 g cm^(−3)),less electrolyte usage,good security for flame retardance,and decent Li-storage behaviors.With lean and LiNO_(3)-free electrolyte,packed full cells exhibit excellent redox kinetics,suppressed LiPS shuttling,and excellent cyclability.This may trigger great research enthusiasm in rational design of low-carbon and safer S cathodes.
基金support from National Natural Science Foundation of China(No.21772188,No.22179109)Chongqing Natural Science Foundation(cstc2021ycjh-bgzxm0164,cstc2020jcyj-zdxmX0010)。
文摘Sulfur and selenium have been paid more and more attention in energy storage systems because of their high theoretical specific gravimetric and volumetric capacities.With the increasing scarcity of lithium resources,secondary batteries made of sulfur and selenium coupled with other alkali metal/alkaline earth metals(e.g.Na,K,Mg)are expected to play a vital role in future production and human life.Due to the volume expansion,poor conductivity and shuttle effect,the structure design of cathode,as one of the important roles in metal-S/Se batteries,has always been a hot and difficult point.In the review,various host materials of S and Se are clarified and discussed.Typically,carbonaceous materials are the most widely used hosts,while polar materials are becoming more and more popular in metal-S/Se batteries.Through a comprehensive overview,it is hoped that previous research experiences can provide further reference and guidance for the sustainable development of metal-S/Se batteries.
文摘With the development of human society and the depletion of non-renewable energy sources,alternate energy resources are becoming an urgent demand.In recent years,energy storage and conversion devices have drawn wide attention as a bridge between sustainable energy sources and daily life.
基金financial supports from National Natural Science Foundation of China (51802269 and 21773138)Chongqing Natural Science Foundation (cstc2018jcyjAX0624)+1 种基金Fundamental Research Funds for the Central Universities (XDJK2019AA002)Venture & Innovation Support Program for Chongqing overseas returnees (cx2018027)。
文摘Smartcombination of manifold carbonaceous materials with admirable functionalities(like full of pores/functional groups,high specific surface area) is still a mainstream/preferential way to address knotty issues of polysulfides dissolution/shuttling and poor electrical conductivity for S-based cathodes.However,extensive use of conductive carbon fillers in cell designs/technology would induce electrolytic overconsumption and thereby shelve high-energy-density promise of Li-S cells.To cut down carbon usage,we propose the incorporation of multi-functionalized NiFe2O4 quantum dots(QDs) as affordable additive substitutes.The total carbon content can be greatly curtailed from 26%(in traditional S/C cathodes) to a low/commercial mass ratio(~5%).Particularly,note that NiFe2O4 QDs additives own superb chemisorption interactions with soluble Li2Sn molecules and proper catalytic features facilitating polysulfide phase conversions and can also strengthen charge-transfer capability/redox kinetics of overall cathode systems.Benefiting from these intrinsic properties,such hybrid cathodes demonstrate prominent rate behaviors(decent capacity retention with ~526 mAh g^-1 even at 5 A g^-1) and stable cyclic performance in LiNO3-free electrolytes(only ~0.08% capacity decay per cycle in 500 cycles at 0.2 A g^-1).This work may arouse tremendous research interest in seeking other alternative QDs and offer an economical/more applicable methodology to construct low-carbon-content electrodes for practical usage.
基金This work is financially supported by Grants from the National Natural Science Foundation of China(No.21773188,21972111,U1530401)Natural Science Foundation of Chongqing(cstc2018jcyjAX0714).
文摘Rechargeable room temperature sodium–sulfur(RT Na–S)batteries are seriously limited by low sulfur utilization and sluggish electrochemical reaction activity of polysulfide intermediates.Herein,a 3D“branch-leaf”biomimetic design proposed for high performance Na–S batteries,where the leaves constructed from Co nanoparticles on carbon nanofibers(CNF)are fully to expose the active sites of Co.The CNF network acts as conductive“branches”to ensure adequate electron and electrolyte supply for the Co leaves.As an effective electrocatalytic battery system,the 3D“branch-leaf”conductive network with abundant active sites and voids can effectively trap polysulfides and provide plentiful electron/ions pathways for electrochemical reaction.DFT calculation reveals that the Co nanoparticles can induce the formation of a unique Co–S–Na molecular layer on the Co surface,which can enable a fast reduction reaction of the polysulfides.Therefore,the prepared“branch-leaf”CNF-L@Co/S electrode exhibits a high initial specific capacity of 1201 mAh g^−1 at 0.1 C and superior rate performance.
基金We appreciate support from the National Natural Science Foundation of China(Nos.22005315 and22179109)Central Universities Fundamental Research Funds(No.SWU-KR22002)Chongqing Natural Science Foundation(No.cstc2020jcyjzdxmX0010).
文摘Although research interest in aqueous metal-sulfur batteries(AMSs)has surged due to their intrinsic low cost and high capacity,the practical application of AMSs remains a considerable challenge because of the restrictive cycling stability.To circumvent this issue,we propose an innovative and simple pre-copper strategy to realize a high-durability aqueous Cu-S battery.The precopper strategy can effectively promote a stable metal dissolution/deposition,compensate for charge carriers,and facilitate reaction kinetics during the subsequent process.As a result,the aqueous Cu-S battery when coupled with S-decorated porous Ti_(3)C_(2)(S-d-Ti_(3)C_(2))exhibits excellent electrochemical performance,delivering a highly reversible capacity of 1805.4 mAh·g^(-1)in the initial cycle at 0.8 A·g^(-1),impressive cycling stability with 90.2%capacity retention over 800 cycles,and ultralow polarization~0.08 V even at a high current density of 3.1 A·g^(-1).The findings obtained in this work could pave the way for the design of highperformance sulfur-based aqueous batteries,which fill the vacancy of the necessary metal anode,delivering merits in both cost and cycle life.
基金The work is supported by the National Natural Science Foundation of China(Nos.11874005,21701153,51601030 and 21773023).
文摘Electrocatalytic water splitting offers a sustainable route for hydrogen production,enabling the clean and renewable alternative energy system of hydrogen economy.The scarcity and high-cost of platinum-group-metal(PGM)materials urge the exploration of high-performance non-PGM electrocatalysts.Herein,a unique hierarchical structure of NiA/2O3 with extraordinary electrocatalytic performance(e.g.t overpotentials as low as 22 mV at 20 mA·cm^-2 and 94 mV at 100 mA·cm^-2)toward hydrogen evolution reaction in alkaline electrolyte(1 M KOH)is reported.The investigation on the hierarchical NiA/2O3 with a bimodal size-distribution also offers insight of interfacial engineering that only proper NiA/2O3 interface can effectively improve H20 adsorption,H20 dissociation as well as H adsorption,for an efficient hydrogen production.