Aqueous zinc-ion batteries possess substantial potential for energy storage applications;however,they are hampered by challenges such as dendrite formation and uncontrolled side reactions occurring at the zinc anode.I...Aqueous zinc-ion batteries possess substantial potential for energy storage applications;however,they are hampered by challenges such as dendrite formation and uncontrolled side reactions occurring at the zinc anode.In our investigation,we sought to mitigate these issues through the utilization of in situ zinc complex formation reactions to engineer hydrophobic protective layers on the zinc anode surface.These robust interfacial layers serve as effective barriers,isolating the zinc anode from the electrolyte and active water molecules and thereby preventing hydrogen evolution and the generation of undesirable byproducts.Additionally,the presence of numerous zincophilic sites within these protective layers facilitates uniform zinc deposition while concurrently inhibiting dendrite growth.Through comprehensive evaluation of functional anodes featuring diverse functional groups and alkyl chain lengths,we meticulously scrutinized the underlying mechanisms influencing performance variations.This analysis involved precise modulation of interfacial hydrophobicity,rapid Zn^(2+)ion transport,and ordered deposition of Zn^(2+)ions.Notably,the optimized anode,fabricated with octadecylphosphate(OPA),demonstrated exceptional performance characteristics.The Zn//Zn symmetric cell exhibited remarkable longevity,exceeding 4000 h under a current density of 2 mA cm^(-2)and a capacity density of 2 mA h cm^(-2),Furthermore,when integrated with a VOH cathode,the complete cell exhibited superior capacity retention compared to anodes modified with alternative organic molecules.展开更多
The number of lithium-ion batteries(LIBs)is steadily increasing in order to meet the ever-growing demand for sustainable energy and a high quality of life for humankind.At the same time,the resulting large number of L...The number of lithium-ion batteries(LIBs)is steadily increasing in order to meet the ever-growing demand for sustainable energy and a high quality of life for humankind.At the same time,the resulting large number of LIB waste certainly poses safety hazards if it is not properly disposed of and will seriously harm the environment due to its inherent toxicity due to the use of toxic substances.Moreover,the consumption of many scarce precious metal resources is behind the mass production of batteries.In the light of severe environmental,resources,safety and recycling problems,recycling spent LIBs have become an essential urgently needed action to achieve sustainable social development.This review therefore critically analyses the value and the need for recycling of spent LIBs from a variety of resources and the environment.A range of existing technologies for recycling and reusing spent LIBs,such as pretreatment,pyrometallurgy,hydrometallurgy,and direct recycled methods,is subsequently summarized exclusively.In addition,the benefits and problems of the methods described above are analyzed in detail.It also introduces recycling progress of other LIB components,such as anodes,separators,and electrolytes,as well as the high-value cathode.Finally,the prospects for recycling LIBs are addressed in four ways(government,users,battery manufacturers,and recyclers).This review should contribute to the development of the recycling of used LIBs,particularly in support of industrialization and recycling processes.展开更多
Zinc metal is a promising anode material for next-generation aqueous batteries,but its practical application is limited by the formation of zinc dendrite.To prevent zinc dendrite growth,various Zn^(2+)-conducting but ...Zinc metal is a promising anode material for next-generation aqueous batteries,but its practical application is limited by the formation of zinc dendrite.To prevent zinc dendrite growth,various Zn^(2+)-conducting but water-isolating solid-electrolyte interphase(SEI)films have been developed,however,the required high-purity chemical materials are extremely expensive.In this work,phosphogypsum(PG),an industrial byproduct produced from the phosphoric acid industry,is employed as a multifunctional protective layer to navigate uniform zinc deposition.Theoretical and experimental results demonstrate that PG-derived CaSO_(4)2H_(2)O can act as an artificial SEI layer to provide fast channels for Zn^(2+)transport.Moreover,CaSO_(4)2H_(2)O could release calcium ions(Ca^(2+))due to its relatively high Kspvalue,which have a higher binding energy than that of Zn^(2+)on the Zn surface,thus preferentially adsorbing to the tips of the protuberances to force zinc ions to nucleate at inert region.As a result,the Zn@PG anode achieves a high Coulombic efficiency of 99.5%during 500 cycles and long-time stability over 1000 hours at 1 m A cm^(-2).Our findings will not only construct a low-cost artificial SEI film for practical metal batteries,but also achieve a high-value utilization of phosphogypsum waste.展开更多
Solid‐state Zn–air batteries(ZABs)hold great potential for application in wearable and flexible electronics.However,further commercialization of current ZABs is still limited by the poor stability and low energy eff...Solid‐state Zn–air batteries(ZABs)hold great potential for application in wearable and flexible electronics.However,further commercialization of current ZABs is still limited by the poor stability and low energy efficiency.It is,thus,crucial to develop efficient catalysts as well as optimize the solid electrolyte system to unveil potential of the ZAB technology.Due to the low cost and versatility in tailoring the structures and properties,carbon materials have been extensively used as the conductive substrates,catalytic air electrodes,and important components in the electrolytes for the solid‐state ZABs.Within this context,we discuss the challenges facing current solid‐state ZABs and summarize the strategies developed to modify properties of carbon‐based electrodes and electrolytes.We highlight the metal−organic framework/covalent organic framework‐based electrodes,heteroatom‐doped carbon,and the composites formed of carbon with metal oxides/sulfides/phosphides.We also briefly discuss the progress of graphene oxide‐based solid electrolyte.展开更多
Hard carbon(HC)is broadly recognized as an exceptionally prospective candidate for the anodes of sodium-ion batteries(SIBs),but their practical implementation faces substantial limitations linked to precursor factors,...Hard carbon(HC)is broadly recognized as an exceptionally prospective candidate for the anodes of sodium-ion batteries(SIBs),but their practical implementation faces substantial limitations linked to precursor factors,such as reduced carbon yield and increased cost.Herein,a cost-effective approach is proposed to prepare a coal-derived HC anode with simple pre-oxidation followed by a post-carbonization process which effectively expands the d_(002)layer spacing,generates closed pores and increases defect sites.Through these modifications,the resulting HC anode attains a delicate equilibrium between plateau capacity and sloping capacity,showcasing a remarkable reversible capacity of 306.3 mAh·g^(-1)at 0.03 A·g^(-1).Furthermore,the produ ced HC exhibits fast reaction kinetics and exceptional rate performance,achieving a capacity of 289 mAh·g^(-1)at 0.1 A·g^(-1),equivalent to~94.5%of that at 0.03 A·g^(-1).When implemented in a full cell configuration,the impressive electrochemical performance is evident,with a notable energy density of 410.6 Wh·kg^(-1)(based on cathode mass).In short,we provide a straightforward yet efficient method for regulating coal-derived HC,which is crucial for the widespread use of SIBs anodes.展开更多
Anions in the electrolyte are usually ignored in conventional"rocking-chair"batteries because only cationic de-/intercalation is considered.An ingenious scheme combining LiMn_(0.7)Fe_(0.3)PO_(4)(LMFP@C)and g...Anions in the electrolyte are usually ignored in conventional"rocking-chair"batteries because only cationic de-/intercalation is considered.An ingenious scheme combining LiMn_(0.7)Fe_(0.3)PO_(4)(LMFP@C)and graphite as a hybrid cathode for lithium-ion batteries(LIBs)is elaborately designed in order to exploit the potential value of anions for battery performance.The hybrid cathode has a higher conductivity and energy density than any of the individual components,allowing for the co-utilization of cations and an-ions through the de-/intercalation of Li^(+)and PF_(6)−over a wide voltage range.The optimal compound with a weight mix ratio of LMFP@C:graphite=5:1 can deliver the highest specific capacity of nearly 140 mA h/g at 0.1 C and the highest voltage plateau of around 4.95 V by adjusting the appropriate mixing ratio.In addition,cyclic voltammetry was used to investigate the electrode kinetics of Li^(+)and PF_(6)−dif-fusion in the hybrid compound at various scan rates.In situ X-ray diffraction is also performed to further demonstrate the structural evolution of the hybrid cathode during the charge/discharge process.展开更多
According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emer...According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emerging technology,indicating its promising development for future energy-storage applications[1].In practical applications,commercialized lithium-ion batteries(LIBs)with lithium cobalt oxide and ternary oxide as cathode materials have assumed a dominant position[2].However,these cathode materials of LIBs are highly dependent on expensive cobalt and nickel,rendering them less sustainable for grid-scale energy storage.Conversely,cathode materials in SIBs appear more sustainable due to their lower dependence on cobalt.Furthermore,the strategic importance of reducing over-dependence on lithium resources cannot be overstated.Hence,SIB technology can serve as one of the potential solutions to mitigate this issue[3].展开更多
The accelerating electrification has sparked an explosion in lithium-ion batteries(LIBs)consumption.As the lifespan declines,the substantial LIBs will flow into the recycling market and promise to spawn a giant recycl...The accelerating electrification has sparked an explosion in lithium-ion batteries(LIBs)consumption.As the lifespan declines,the substantial LIBs will flow into the recycling market and promise to spawn a giant recycling system.Nonetheless,since the lack of unified guiding standard and nontraceability,the recycling of end-of-life LIBs has fallen into the dilemma of low recycling rate,poor recycling efficiency,and insignificant benefits.Herein,tapping into summarizing and analyzing the current status and challenges of recycling LIBs,this outlook provides insights for the future course of full lifecycle management of LIBs,proposing gradient utilization and recycling-target predesign strategy.Further,we acknowledge some recommendations for recycling waste LIBs and anticipate a collaborative effort to advance sustainable and reliable recycling routes.展开更多
基金financially supported by the Jiangsu Distinguished Professors Project (No.1711510024)the Funding for Scientific Research Startup of Jiangsu University (No.4111510015,19JDG044)+5 种基金the Jiangsu Provincial Program for High-Level Innovative and Entrepreneurial Talents Introductionthe National Natural Science Foundation of China (No.22008091)the Jiangsu Agriculture Science and Technology Innovation Fund (No.CX (21)1007)the Natural Science Foundation of Guangdong Province (2023A1515010894)the Open Project of Luzhou Key Laboratory of Fine Chemical Application Technology (HYJH-2302-A)the National Institute of Education,Singapore,under its Academic Research Fund (RI 1/21 EAH)。
文摘Aqueous zinc-ion batteries possess substantial potential for energy storage applications;however,they are hampered by challenges such as dendrite formation and uncontrolled side reactions occurring at the zinc anode.In our investigation,we sought to mitigate these issues through the utilization of in situ zinc complex formation reactions to engineer hydrophobic protective layers on the zinc anode surface.These robust interfacial layers serve as effective barriers,isolating the zinc anode from the electrolyte and active water molecules and thereby preventing hydrogen evolution and the generation of undesirable byproducts.Additionally,the presence of numerous zincophilic sites within these protective layers facilitates uniform zinc deposition while concurrently inhibiting dendrite growth.Through comprehensive evaluation of functional anodes featuring diverse functional groups and alkyl chain lengths,we meticulously scrutinized the underlying mechanisms influencing performance variations.This analysis involved precise modulation of interfacial hydrophobicity,rapid Zn^(2+)ion transport,and ordered deposition of Zn^(2+)ions.Notably,the optimized anode,fabricated with octadecylphosphate(OPA),demonstrated exceptional performance characteristics.The Zn//Zn symmetric cell exhibited remarkable longevity,exceeding 4000 h under a current density of 2 mA cm^(-2)and a capacity density of 2 mA h cm^(-2),Furthermore,when integrated with a VOH cathode,the complete cell exhibited superior capacity retention compared to anodes modified with alternative organic molecules.
基金financially supported by the National Natural Science Foundation of China(No.52173246)the 111 Project(B13013).
文摘The number of lithium-ion batteries(LIBs)is steadily increasing in order to meet the ever-growing demand for sustainable energy and a high quality of life for humankind.At the same time,the resulting large number of LIB waste certainly poses safety hazards if it is not properly disposed of and will seriously harm the environment due to its inherent toxicity due to the use of toxic substances.Moreover,the consumption of many scarce precious metal resources is behind the mass production of batteries.In the light of severe environmental,resources,safety and recycling problems,recycling spent LIBs have become an essential urgently needed action to achieve sustainable social development.This review therefore critically analyses the value and the need for recycling of spent LIBs from a variety of resources and the environment.A range of existing technologies for recycling and reusing spent LIBs,such as pretreatment,pyrometallurgy,hydrometallurgy,and direct recycled methods,is subsequently summarized exclusively.In addition,the benefits and problems of the methods described above are analyzed in detail.It also introduces recycling progress of other LIB components,such as anodes,separators,and electrolytes,as well as the high-value cathode.Finally,the prospects for recycling LIBs are addressed in four ways(government,users,battery manufacturers,and recyclers).This review should contribute to the development of the recycling of used LIBs,particularly in support of industrialization and recycling processes.
基金financially supported by the National Natural Science Foundation of China (22279122,52042403)the Zhejiang Provincial Natural Science Foundation of China (LZ22B030004)+2 种基金the Ministry of Education,Singapore,under its Academic Research Fund Tier 1 (RG10/22)the National Institute of Education,Singapore,under its Academic Research Fund (RI 1/21 EAH)National Institute of Education,Singapore,under its Start-Up Grant (NIE-SUG4/20AHX)。
文摘Zinc metal is a promising anode material for next-generation aqueous batteries,but its practical application is limited by the formation of zinc dendrite.To prevent zinc dendrite growth,various Zn^(2+)-conducting but water-isolating solid-electrolyte interphase(SEI)films have been developed,however,the required high-purity chemical materials are extremely expensive.In this work,phosphogypsum(PG),an industrial byproduct produced from the phosphoric acid industry,is employed as a multifunctional protective layer to navigate uniform zinc deposition.Theoretical and experimental results demonstrate that PG-derived CaSO_(4)2H_(2)O can act as an artificial SEI layer to provide fast channels for Zn^(2+)transport.Moreover,CaSO_(4)2H_(2)O could release calcium ions(Ca^(2+))due to its relatively high Kspvalue,which have a higher binding energy than that of Zn^(2+)on the Zn surface,thus preferentially adsorbing to the tips of the protuberances to force zinc ions to nucleate at inert region.As a result,the Zn@PG anode achieves a high Coulombic efficiency of 99.5%during 500 cycles and long-time stability over 1000 hours at 1 m A cm^(-2).Our findings will not only construct a low-cost artificial SEI film for practical metal batteries,but also achieve a high-value utilization of phosphogypsum waste.
基金This study was financially supported by the National Key R&D Research Program of China(Grant No.2018YFB0905400)National Natural Science Foundationof China(Grant Nos.,51925207,U1910210,51972067,51802044,and 51872277)+2 种基金Guangdong Natural Science Funds for Distinguished Young Scholar(Grant No.2019B151502039)Fundamental Research Funds for the Central Universities of China(Grant No.WK2060140026)the DNL Cooperation Fund,CAS(Grant No.DNL180310).
文摘Solid‐state Zn–air batteries(ZABs)hold great potential for application in wearable and flexible electronics.However,further commercialization of current ZABs is still limited by the poor stability and low energy efficiency.It is,thus,crucial to develop efficient catalysts as well as optimize the solid electrolyte system to unveil potential of the ZAB technology.Due to the low cost and versatility in tailoring the structures and properties,carbon materials have been extensively used as the conductive substrates,catalytic air electrodes,and important components in the electrolytes for the solid‐state ZABs.Within this context,we discuss the challenges facing current solid‐state ZABs and summarize the strategies developed to modify properties of carbon‐based electrodes and electrolytes.We highlight the metal−organic framework/covalent organic framework‐based electrodes,heteroatom‐doped carbon,and the composites formed of carbon with metal oxides/sulfides/phosphides.We also briefly discuss the progress of graphene oxide‐based solid electrolyte.
基金financially supported by the National Natural Science Foundation of China(No.52173246)111 project(No.B13013)Shccig-Qinling Program(No.SMYJY20220574)。
文摘Hard carbon(HC)is broadly recognized as an exceptionally prospective candidate for the anodes of sodium-ion batteries(SIBs),but their practical implementation faces substantial limitations linked to precursor factors,such as reduced carbon yield and increased cost.Herein,a cost-effective approach is proposed to prepare a coal-derived HC anode with simple pre-oxidation followed by a post-carbonization process which effectively expands the d_(002)layer spacing,generates closed pores and increases defect sites.Through these modifications,the resulting HC anode attains a delicate equilibrium between plateau capacity and sloping capacity,showcasing a remarkable reversible capacity of 306.3 mAh·g^(-1)at 0.03 A·g^(-1).Furthermore,the produ ced HC exhibits fast reaction kinetics and exceptional rate performance,achieving a capacity of 289 mAh·g^(-1)at 0.1 A·g^(-1),equivalent to~94.5%of that at 0.03 A·g^(-1).When implemented in a full cell configuration,the impressive electrochemical performance is evident,with a notable energy density of 410.6 Wh·kg^(-1)(based on cathode mass).In short,we provide a straightforward yet efficient method for regulating coal-derived HC,which is crucial for the widespread use of SIBs anodes.
基金financially supported by the National Natural Science Foundation of China(No.91963118,and No.52173246)the Science Technology Program of Jilin Province(No.20200201066JC)the 111 Project(No.B13013)。
文摘Anions in the electrolyte are usually ignored in conventional"rocking-chair"batteries because only cationic de-/intercalation is considered.An ingenious scheme combining LiMn_(0.7)Fe_(0.3)PO_(4)(LMFP@C)and graphite as a hybrid cathode for lithium-ion batteries(LIBs)is elaborately designed in order to exploit the potential value of anions for battery performance.The hybrid cathode has a higher conductivity and energy density than any of the individual components,allowing for the co-utilization of cations and an-ions through the de-/intercalation of Li^(+)and PF_(6)−over a wide voltage range.The optimal compound with a weight mix ratio of LMFP@C:graphite=5:1 can deliver the highest specific capacity of nearly 140 mA h/g at 0.1 C and the highest voltage plateau of around 4.95 V by adjusting the appropriate mixing ratio.In addition,cyclic voltammetry was used to investigate the electrode kinetics of Li^(+)and PF_(6)−dif-fusion in the hybrid compound at various scan rates.In situ X-ray diffraction is also performed to further demonstrate the structural evolution of the hybrid cathode during the charge/discharge process.
基金supported by the National Key R&D Program of China(2023YFE0202000)the National Natural Science Foundation of China(52173246)Double-Thousand Talents Plan of Jiangxi Province(jxsq2023102005)。
文摘According to the reports of"Top Ten Emerging Technologies in Chemistry 2022"released by the International Union of Pure and Applied Chemistry,sodium-ion battery(SIB)technology is identified as a crucial emerging technology,indicating its promising development for future energy-storage applications[1].In practical applications,commercialized lithium-ion batteries(LIBs)with lithium cobalt oxide and ternary oxide as cathode materials have assumed a dominant position[2].However,these cathode materials of LIBs are highly dependent on expensive cobalt and nickel,rendering them less sustainable for grid-scale energy storage.Conversely,cathode materials in SIBs appear more sustainable due to their lower dependence on cobalt.Furthermore,the strategic importance of reducing over-dependence on lithium resources cannot be overstated.Hence,SIB technology can serve as one of the potential solutions to mitigate this issue[3].
基金National Natural Science Foundation of China,Grant/Award Numbers:52173246,91963118。
文摘The accelerating electrification has sparked an explosion in lithium-ion batteries(LIBs)consumption.As the lifespan declines,the substantial LIBs will flow into the recycling market and promise to spawn a giant recycling system.Nonetheless,since the lack of unified guiding standard and nontraceability,the recycling of end-of-life LIBs has fallen into the dilemma of low recycling rate,poor recycling efficiency,and insignificant benefits.Herein,tapping into summarizing and analyzing the current status and challenges of recycling LIBs,this outlook provides insights for the future course of full lifecycle management of LIBs,proposing gradient utilization and recycling-target predesign strategy.Further,we acknowledge some recommendations for recycling waste LIBs and anticipate a collaborative effort to advance sustainable and reliable recycling routes.