Lithium metal is considered the ideal anode material for Li-ion-based batteries because it exhibits the highest specific capacity and lowest redox potential for this type of cells. However, growth of Li dendrites, uns...Lithium metal is considered the ideal anode material for Li-ion-based batteries because it exhibits the highest specific capacity and lowest redox potential for this type of cells. However, growth of Li dendrites, unstable solid electrolyte interphases, low Coulombic efficiencies, and safety hazards have significantly hindered the practical application of metallic Li anodes. Herein, we propose a three-dimensional （3D） carbon nanotube sponge （CNTS） as a Li deposition host. The high specific surface area of the CNTS enables homogenous charge distribution for Li nucleation and minimizes the effective current density to overcome dendrite growth. An additional conformal A1203 layer on the CNTS coated by atomic layer deposition （ALD） robustly protects the Li metal electrode/electrolyte interface due to the good chemical stability and high mechanical strength of the layer. The Li@ALD-CNTS electrode exhibits stable voltage profiles with a small overpotential ranging from 16 to 30 mV over 100 h of cycling at 1.0 mA·cm^-2. Moreover, the electrodes display a dendrite-free morphology after cycling and a Coulombic efficiency of 92.4% over 80 cycles at 1.0 mA·cm^-2 in an organic carbonate electrolyte, thus demonstrating electrochemical stability superior to that of planar current collectors. Our results provide an important strategy for the rational design of current collectors to obtain stable Li metal anodes.展开更多
Lithium metal has been regarded as one of the most promising anode materials for high-energy-density batteries due to its extremely high theoretical gravimetric capacity of 3860 mAh·g^-1 along with its low electr...Lithium metal has been regarded as one of the most promising anode materials for high-energy-density batteries due to its extremely high theoretical gravimetric capacity of 3860 mAh·g^-1 along with its low electrochemical potential of-3.04 V.Unfortunately,uncontrollable Li dendrite growth and repetitive destruction/formation of the solid electrolyte interphase layer lead to poor safety and low Coulombic efficiencies(CEs)for long-term utilization,which largely restricts the practical applications of lithium metal anode.In this review,we comprehensively summarized important progresses achieved to date in suppressing Li dendrite growth.Strategies for protection of Li metal anodes include designing porous structured hosts,fabricating artificial solid electrolyte interface(SEI)layers,introducing electrolyte additives,using solid-state electrolytes and applying external fields.The protection of Li metal anodes can be achieved by regulating the stripping and deposition behaviours of Li ions.Finally,the challenges remaining for lithium metal battery systems and future perspectives for Li metal anodes in practical applications are outlined,which are expected to shed light on future research in this field.展开更多
Featured with high power density,improved safety and low-cost,rechargeable aqueous zinc-ion batteries(ZIBs) have been revived as possible candidates for sustainable energy storage systems in recent years.However,the c...Featured with high power density,improved safety and low-cost,rechargeable aqueous zinc-ion batteries(ZIBs) have been revived as possible candidates for sustainable energy storage systems in recent years.However,the challenges inherent in zinc(Zn) anode,namely dendrite formation and interfacial parasitic reactions,have greatly impeded their practical application.Whereas the critical issue of dendrite formation has attracted widespread concern,the parasitic reactions of Zn anodes with mildly acidic electrolytes have received very little attentions.Considering that the low Zn reversibility that stems from interfacial parasitic reactions is the major obstacle to the commercialization of ZIBs,thorough understanding of these side reactions and the development of correlative inhibition strategies are significant.Therefore,in this review,the brief fundamentals of corrosion and hydrogen evolution reactions at Zn surface is presented.In addition,recent advances and research efforts addressing detrimental side reactions are reviewed from the perspective of electrode design,electrode-electrolyte interfacial engineering and electrolyte modification.To facilitate the future researches on this aspect,perspectives and suggestions for relevant investigations are provided lastly.展开更多
为了满足储能市场对高功率电池的需求,开发具有高功率性能的锂离子电池负极材料成为必然发展趋势。本文通过湿式合成法将软碳和硬碳的前驱体进行复合,开发了一种新型的复合碳锂离子电池负极材料。考察了其克比容量、库仑效率、倍率性能...为了满足储能市场对高功率电池的需求,开发具有高功率性能的锂离子电池负极材料成为必然发展趋势。本文通过湿式合成法将软碳和硬碳的前驱体进行复合,开发了一种新型的复合碳锂离子电池负极材料。考察了其克比容量、库仑效率、倍率性能以及循环稳定性。用X射线粉末衍射(XRD)、拉曼、扫描电镜(SEM)以及透射电子显微镜(TEM)对所制备的复合碳材料的结构和表面形貌进行表征。结果表明,该复合碳材料同时具有软碳和硬碳的优点,且性能优于机械混合碳,在保持高比容量和高效率的前提下,倍率性能尤为突出,其2C容量可达154 m A·h/g,且2C/0.2C的容量保持率为64.2%;同时0.2C克比容量为240 m A·h/g,库仑效率为82%。经过5C充放电后,恢复0.2C小电流充放电后,容量保持率达99.8%,循环稳定性很好。XRD、拉曼以及透射电子显微镜的表征结果均表明软、硬碳在复合过程中不只是简单机械共混而是具有协同效应。展开更多
Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synth...Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synthesis and low yield of nanoporous silicon limit its practical application.Here,we develop a scalable,low-cost top-down process of controlled oxidation of Mg2Si in the air,followed by HCl removal of MgO to generate nanoporous silicon without the use of HF.By controlling the synthesis conditions,the oxygen content,grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints.In situ environmental transmission electron microscopy reveals the reaction mechanism;the Mg2Si microparticle reacts with O2 to form MgO and Si,while preventing SiO2 formation.Owing to the low oxygen content and microscale secondary structure,the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles(3,033 mAh/g vs.2,418 mAh/g,84.3%vs.73.1%).Synthesis is highly scalable,and a yield of 90.4%is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch.Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.展开更多
Lithium-sulfur(Li-S)battery is recognized as one of the promising candidates to break through the specific energy limitations of commercial lithium-ion batteries given the high theoretical specific energy,environmenta...Lithium-sulfur(Li-S)battery is recognized as one of the promising candidates to break through the specific energy limitations of commercial lithium-ion batteries given the high theoretical specific energy,environmental friendliness,and low cost.Over the past decade,tremendous progress have been achieved in improving the electrochemical performance especially the lifespan by various strategies mainly concentrated on the sulfur cathodes.In this review,the fundamental electrochemistry of sulfur cathode and lithium anode is revealed to understand the current dilemmas.And the advances achieved through diverse strategies are comprehensively summarized,which involves lithium polysulfides(LiPSs)limitation,sulfur redox reaction regulation and electrocatalysis in sulfur cathode and artificial solid electrolyte interface(SEI),electrolyte design,and structured anode in lithium anode.Additionally,the differences between laboratory level coin cells and actual pouch cells need to be addressed that only few reports on practical Li-S pouch cell are available due to the unexpected problems on both sulfur cathode and lithium anode which are masked at lithium and electrolyte excess.Lastly,the challenges and perspective toward the practical Li-S batteries are also offered.展开更多
Li metal has been regarded as one of the most promising anodes for high-energy-density storage systems due to its high theoretical capacity and lowest electrochemical potential.Unfortunately,an unstable and non-unifor...Li metal has been regarded as one of the most promising anodes for high-energy-density storage systems due to its high theoretical capacity and lowest electrochemical potential.Unfortunately,an unstable and non-uniform solid electrolyte interphase(SEI)deriving from the spontaneous reaction between Li metal anode and electrolyte causes uneven Li deposition,resulting in the growth of Li dendrites and low Coulombic efficiency,which have greatly hindered the practical application of Li metal batteries.Thus,the construction of a stable SEI is an effective approach to suppress the growth of Li dendrites and enhance the electrochemical performances of Li metal anode.In this review,we firstly introduce the formation process of inferior SEI of Li metal anode and the corresponding challenges caused by the unstable SEI.Next,recent progresses to modify SEI layer through the regulation of electrolyte compositions and exsitu protective coating are summarized.Finally,the remained issues,challenges,and perspectives are also proposed on the basis of current research status and progress.展开更多
Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in th...Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in the battery so that the lithium loss during the first charge and long-term cycling can be compensated.Such an effect does not need to change the major electrode material or battery structure and is compatible with the majority of current lithium-ion battery production lines.At this stage,various prelithiation methods have been reported,some of which are already in the pilot-scale production stage.But there is still no definitive development roadmap for prelithiation.In this review,we first introduce the influence of prelithiation on electrochemical performance from a theoretical point of view and then compare the pros and cons of different prelithiation methods in different battery manufacturing stages.Finally,we discuss the challenges and future development trends of prelithiation.We aim to build up a bridge between academic research and industrial application.Some engineering problems in the promotion of prelithiation technique are extensively discussed,including not only the implementation of prelithiation but also some collateral issues on battery designing and management.展开更多
Due to the abundant sodium reserves and high safety,sodium ion batteries(SIBs)are foreseen a promising future.While,hard carbon materials are very suitable for the anode of SIBs owing to their structure and cost advan...Due to the abundant sodium reserves and high safety,sodium ion batteries(SIBs)are foreseen a promising future.While,hard carbon materials are very suitable for the anode of SIBs owing to their structure and cost advantages.However,the unsatisfactory initial coulombic efficiency(ICE)is one of the crucial blemishes of hard carbon materials and the slow sodium storage kinetics also hinders their wide application.Herein,with spherical nano SiO_(2)as pore-forming agent,gelatin and polytetrafluoroethylene as carbon sources,a multi-porous carbon(MPC)material can be easily obtained via a co-pyrolysis method,by which carbonization and template removal can be achieved synchronously without the assistance of strong acids or strong bases.As a result,the MPC anode exhibited remarkable ICE of 83%and a high rate capability(208 m Ah/g at 5 A/g)when used in sodium-ion half cells.Additionally,coupling with Na3V2(PO4)3as the cathode to assemble full cells,the as-fabricated MPC//NVP full cell delivered a good rate capability(146 m Ah/g at 5 A/g)as well,implying a good application prospect the MPC anode has.展开更多
文摘Lithium metal is considered the ideal anode material for Li-ion-based batteries because it exhibits the highest specific capacity and lowest redox potential for this type of cells. However, growth of Li dendrites, unstable solid electrolyte interphases, low Coulombic efficiencies, and safety hazards have significantly hindered the practical application of metallic Li anodes. Herein, we propose a three-dimensional （3D） carbon nanotube sponge （CNTS） as a Li deposition host. The high specific surface area of the CNTS enables homogenous charge distribution for Li nucleation and minimizes the effective current density to overcome dendrite growth. An additional conformal A1203 layer on the CNTS coated by atomic layer deposition （ALD） robustly protects the Li metal electrode/electrolyte interface due to the good chemical stability and high mechanical strength of the layer. The Li@ALD-CNTS electrode exhibits stable voltage profiles with a small overpotential ranging from 16 to 30 mV over 100 h of cycling at 1.0 mA·cm^-2. Moreover, the electrodes display a dendrite-free morphology after cycling and a Coulombic efficiency of 92.4% over 80 cycles at 1.0 mA·cm^-2 in an organic carbonate electrolyte, thus demonstrating electrochemical stability superior to that of planar current collectors. Our results provide an important strategy for the rational design of current collectors to obtain stable Li metal anodes.
基金the financial support from the National Natural Science Foundation of China(51831009)the National Materials Genome Project(2016YFB0700600)the National Youth Top-Notch Talent Support Program。
文摘Lithium metal has been regarded as one of the most promising anode materials for high-energy-density batteries due to its extremely high theoretical gravimetric capacity of 3860 mAh·g^-1 along with its low electrochemical potential of-3.04 V.Unfortunately,uncontrollable Li dendrite growth and repetitive destruction/formation of the solid electrolyte interphase layer lead to poor safety and low Coulombic efficiencies(CEs)for long-term utilization,which largely restricts the practical applications of lithium metal anode.In this review,we comprehensively summarized important progresses achieved to date in suppressing Li dendrite growth.Strategies for protection of Li metal anodes include designing porous structured hosts,fabricating artificial solid electrolyte interface(SEI)layers,introducing electrolyte additives,using solid-state electrolytes and applying external fields.The protection of Li metal anodes can be achieved by regulating the stripping and deposition behaviours of Li ions.Finally,the challenges remaining for lithium metal battery systems and future perspectives for Li metal anodes in practical applications are outlined,which are expected to shed light on future research in this field.
基金financially supported by the National Key R&D Program of China (grant no. 2018YFB0905400)the National Natural Science Foundation of China (grant nos. 22075331, 51702376, 21905057)+2 种基金the Fundamental Research Funds for the Central Universities (19lgzd02)the Guangdong Pearl River Talents Plan (2019QN01L117)the National Thousand Youth Talents Project of the Chinese Government.
文摘Featured with high power density,improved safety and low-cost,rechargeable aqueous zinc-ion batteries(ZIBs) have been revived as possible candidates for sustainable energy storage systems in recent years.However,the challenges inherent in zinc(Zn) anode,namely dendrite formation and interfacial parasitic reactions,have greatly impeded their practical application.Whereas the critical issue of dendrite formation has attracted widespread concern,the parasitic reactions of Zn anodes with mildly acidic electrolytes have received very little attentions.Considering that the low Zn reversibility that stems from interfacial parasitic reactions is the major obstacle to the commercialization of ZIBs,thorough understanding of these side reactions and the development of correlative inhibition strategies are significant.Therefore,in this review,the brief fundamentals of corrosion and hydrogen evolution reactions at Zn surface is presented.In addition,recent advances and research efforts addressing detrimental side reactions are reviewed from the perspective of electrode design,electrode-electrolyte interfacial engineering and electrolyte modification.To facilitate the future researches on this aspect,perspectives and suggestions for relevant investigations are provided lastly.
文摘为了满足储能市场对高功率电池的需求,开发具有高功率性能的锂离子电池负极材料成为必然发展趋势。本文通过湿式合成法将软碳和硬碳的前驱体进行复合,开发了一种新型的复合碳锂离子电池负极材料。考察了其克比容量、库仑效率、倍率性能以及循环稳定性。用X射线粉末衍射(XRD)、拉曼、扫描电镜(SEM)以及透射电子显微镜(TEM)对所制备的复合碳材料的结构和表面形貌进行表征。结果表明,该复合碳材料同时具有软碳和硬碳的优点,且性能优于机械混合碳,在保持高比容量和高效率的前提下,倍率性能尤为突出,其2C容量可达154 m A·h/g,且2C/0.2C的容量保持率为64.2%;同时0.2C克比容量为240 m A·h/g,库仑效率为82%。经过5C充放电后,恢复0.2C小电流充放电后,容量保持率达99.8%,循环稳定性很好。XRD、拉曼以及透射电子显微镜的表征结果均表明软、硬碳在复合过程中不只是简单机械共混而是具有协同效应。
基金This work was supported by Samsung SDI.Part of this work was performed at the Stanford Nano Shared Facilities(SNSF)Stanford Nanofabrication Facility(SNF).
文摘Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials.However,the high cost of synthesis and low yield of nanoporous silicon limit its practical application.Here,we develop a scalable,low-cost top-down process of controlled oxidation of Mg2Si in the air,followed by HCl removal of MgO to generate nanoporous silicon without the use of HF.By controlling the synthesis conditions,the oxygen content,grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints.In situ environmental transmission electron microscopy reveals the reaction mechanism;the Mg2Si microparticle reacts with O2 to form MgO and Si,while preventing SiO2 formation.Owing to the low oxygen content and microscale secondary structure,the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles(3,033 mAh/g vs.2,418 mAh/g,84.3%vs.73.1%).Synthesis is highly scalable,and a yield of 90.4%is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch.Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.
基金supported by the fellowship of the National Natural Science Foundation of China(No.22209177)the China Postdoctoral Science Foundation(No.2021M703149)+2 种基金the Strategy Priority Research Program of Chinese Academy of Science(No.XDA17020404)the R&D Projects in Key Areas of Guangdong Province(No.2019B090908001)the High-Specific-Energy Primary Power Battery Project(No.2020-PYS/KYY-J033).
文摘Lithium-sulfur(Li-S)battery is recognized as one of the promising candidates to break through the specific energy limitations of commercial lithium-ion batteries given the high theoretical specific energy,environmental friendliness,and low cost.Over the past decade,tremendous progress have been achieved in improving the electrochemical performance especially the lifespan by various strategies mainly concentrated on the sulfur cathodes.In this review,the fundamental electrochemistry of sulfur cathode and lithium anode is revealed to understand the current dilemmas.And the advances achieved through diverse strategies are comprehensively summarized,which involves lithium polysulfides(LiPSs)limitation,sulfur redox reaction regulation and electrocatalysis in sulfur cathode and artificial solid electrolyte interface(SEI),electrolyte design,and structured anode in lithium anode.Additionally,the differences between laboratory level coin cells and actual pouch cells need to be addressed that only few reports on practical Li-S pouch cell are available due to the unexpected problems on both sulfur cathode and lithium anode which are masked at lithium and electrolyte excess.Lastly,the challenges and perspective toward the practical Li-S batteries are also offered.
基金financially supported by the National Natural Science Foundation of China(Grant no.51678182)China Postdoctoral Science Foundation(Grant no.2019M650663)Start-up Grant of Harbin Institute of Technology,Shenzhen。
文摘Li metal has been regarded as one of the most promising anodes for high-energy-density storage systems due to its high theoretical capacity and lowest electrochemical potential.Unfortunately,an unstable and non-uniform solid electrolyte interphase(SEI)deriving from the spontaneous reaction between Li metal anode and electrolyte causes uneven Li deposition,resulting in the growth of Li dendrites and low Coulombic efficiency,which have greatly hindered the practical application of Li metal batteries.Thus,the construction of a stable SEI is an effective approach to suppress the growth of Li dendrites and enhance the electrochemical performances of Li metal anode.In this review,we firstly introduce the formation process of inferior SEI of Li metal anode and the corresponding challenges caused by the unstable SEI.Next,recent progresses to modify SEI layer through the regulation of electrolyte compositions and exsitu protective coating are summarized.Finally,the remained issues,challenges,and perspectives are also proposed on the basis of current research status and progress.
基金National Natural Science Foundation of China,Grant/Award Numbers:22179045,5202780089。
文摘Prelithiation technology is widely considered a feasible route to raise the energy density and elongate the cycle life of lithium-ion batteries.The principle of prelithiation is to introduce extra active Li ions in the battery so that the lithium loss during the first charge and long-term cycling can be compensated.Such an effect does not need to change the major electrode material or battery structure and is compatible with the majority of current lithium-ion battery production lines.At this stage,various prelithiation methods have been reported,some of which are already in the pilot-scale production stage.But there is still no definitive development roadmap for prelithiation.In this review,we first introduce the influence of prelithiation on electrochemical performance from a theoretical point of view and then compare the pros and cons of different prelithiation methods in different battery manufacturing stages.Finally,we discuss the challenges and future development trends of prelithiation.We aim to build up a bridge between academic research and industrial application.Some engineering problems in the promotion of prelithiation technique are extensively discussed,including not only the implementation of prelithiation but also some collateral issues on battery designing and management.
基金financially supported by the Start-up Funding of Jinan University(No.88016105)the Discipline Construction Outstanding Young Backbone Project(No.12819023)+3 种基金the Fundamental Research Funds for the Central Universities(No.21620317)the Guangdong Basic and Applied Basic Research Foundation(Nos.2020A1515110611 and 2021A1515010362)the Guangzhou Basic and Applied Basic Research Foundation(No.202102020995)supported by the Open Fund of Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications(No.2020B121201005)。
文摘Due to the abundant sodium reserves and high safety,sodium ion batteries(SIBs)are foreseen a promising future.While,hard carbon materials are very suitable for the anode of SIBs owing to their structure and cost advantages.However,the unsatisfactory initial coulombic efficiency(ICE)is one of the crucial blemishes of hard carbon materials and the slow sodium storage kinetics also hinders their wide application.Herein,with spherical nano SiO_(2)as pore-forming agent,gelatin and polytetrafluoroethylene as carbon sources,a multi-porous carbon(MPC)material can be easily obtained via a co-pyrolysis method,by which carbonization and template removal can be achieved synchronously without the assistance of strong acids or strong bases.As a result,the MPC anode exhibited remarkable ICE of 83%and a high rate capability(208 m Ah/g at 5 A/g)when used in sodium-ion half cells.Additionally,coupling with Na3V2(PO4)3as the cathode to assemble full cells,the as-fabricated MPC//NVP full cell delivered a good rate capability(146 m Ah/g at 5 A/g)as well,implying a good application prospect the MPC anode has.
