Recycling useful materials such as Ag, Al, Sn, Cu and Si from waste silicon solar cell chips is a sustainable project to slow down the ever-growing amount of waste crystalline-silicon photovoltaic panels. However, the...Recycling useful materials such as Ag, Al, Sn, Cu and Si from waste silicon solar cell chips is a sustainable project to slow down the ever-growing amount of waste crystalline-silicon photovoltaic panels. However, the recovery cost of the above-mentioned materials from silicon chips via acid-alkaline treatments outweights the gain economically.Herein, we propose a new proof-of-concept to fabricate Si-based anodes with waste silicon chips as raw materials.Nanoparticles from waste silicon chips were prepared with the high-energy ball milling followed by introducing carbon nanotubes and N-doped carbon into the nanoparticles, which amplifies the electrochemical properties. It is explored that Al and Ag elements influenced electrochemical performance respectively. The results showed that the Al metal in the composite possesses an adverse impact on the electrochemical performance. After removing Al, the composite was confirmed to possess a pronounced durable cycling property due to the presence of Ag, resulting in significantly more superior property than the composite having both Al and Ag removed.展开更多
Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion...Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion batteries.The major bottleneck for SiO/Gr composite anode is the poor cyclability arising from the stress/strain behaviors due to the mismatch between two heterogenous materials during the lithiation/delithiation process.To date,a meticulous and quantitative understanding of the highly nonlinear coupling behaviors of such materials is still lacking.Herein,an electro–chemo–mechanics-coupled detailed model containing particle geometries is established.The underlying mechanism of the regulation between SiO and Gr components during electrochemical cycling is quantitatively revealed.We discover that increasing the SiO weight percentage(wt%)reduces the utilization efficiency of the active materials at the same 1C rate charging and enhances the hindering effects of stress-driven flux on diffusion.In addition,the mechanical constraint demonstrates a balanced effect on the overall performance of cells and the local behaviors of particles.This study provides new insights into the fundamental interactions between SiO and Gr materials and advances the investigation methodology for the design and evaluation of next-generation high-energydensity batteries.展开更多
Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes th...Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.展开更多
SiOx is attractive as an anode material for lithium-ion batteries(LIBs)due to its high capacity,low cost,and relatively higher cyclic stability than Si anode.However,the intrinsic low electronic conductivity,low initi...SiOx is attractive as an anode material for lithium-ion batteries(LIBs)due to its high capacity,low cost,and relatively higher cyclic stability than Si anode.However,the intrinsic low electronic conductivity,low initial coulombic efficiency(ICE),and volume expansion during cycles hinder its applications.In this review,we summarize advances in high performance SiOx anodes,mainly from two aspects:active material and binders.The future perspective is investigated at the end of this review.Our review provides strategical guidance for developing high performance SiOx anodes.展开更多
Implementing high-performance silicon(Si)anode in actual processing and application is highly desirable for next-generation,high-energy Li-ion batteries.However,high content of inactive matrix(including conductive age...Implementing high-performance silicon(Si)anode in actual processing and application is highly desirable for next-generation,high-energy Li-ion batteries.However,high content of inactive matrix(including conductive agent and binder)is often indispensable in order to ensure local conductivity and suppress pulverization tendency of Si particles,which thus cause great capacity loss based on the mass of whole electrode.Here,we designed an accordion-structured,high-performance electrode with high Si content up to 95%.Si nanoparticles were well anchored into the interlayer spacings of accordion-like graphene arrays,and free-standing electrode was prepared via a simple filtration process without any binder.Conductive accordion framework ensures strong confinement effect of Si nanoparticles and also provides direct,non-tortuous channels for fast electrochemical reaction kinetics.As a consequence,the accordion Si electrodes exhibit ultrahigh,electrode-based capacities up to 3149 mAh g^(-1)(under Si content of 91%),as well as long-term stability.Also,the accordion electrode can bear extreme condition of over-lithiation and maintains stable in full-cell test.This design provides a significant stride in high Si content toward realistic,high-performance electrodes.展开更多
Low-cost silicon microparticles(SiMP),as a substitute for nanostructured silicon,easily suffer from cracks and fractured during the electrochemical cycle.A novel n-type conductive polymer binder with excellent electro...Low-cost silicon microparticles(SiMP),as a substitute for nanostructured silicon,easily suffer from cracks and fractured during the electrochemical cycle.A novel n-type conductive polymer binder with excellent electronic and ionic conductivities as well as good adhesion,has been successfully designed and applied for high-performance SiMP anodes in lithium-ion batteries to address this problem.Its unique features are attributed to the stro ng electron-withdrawing oxadiazole ring structure with sulfonate polar groups.The combination of rigid and flexible components in the polymer ensures its good mechanical strength and ductility,which is beneficial to suppress the expansion and contraction of SiMP s during the charge/discharge process.By fine-tuning the monomer ratio,the conjugation and sulfonation degrees of the polymer can be precisely controlled to regulate its ionic and electronic conductivities,which has been systematically analyzed with the help of an electrochemical test method,filling in the gap on the conductivity measurement of the polymer in the doping state.The experimental results indicate that the cell with the developed n-type polymer binder and SiMP(~0.5 μm) anodes achieves much better cycling performance than traditional non-conductive binders.It has been considered that the initial capacity of the SiMP anode is controlled by the synergetic effect of ionic and electronic conductivity of the binder,and the capacity retention mainly depends on its electronic conductivity when the ionic conductivity is sufficient.It is worth noting that the fundamental research of this wo rk is also applicable to other battery systems using conductive polymers in order to achieve high energy density,broadening their practical applications.展开更多
A dual-shell Si/TiO2/CFs composite was synthesized through a simple method to deal with the intrinsic drawbacks of silicon-based anode,in terms of huge volume change,unstable SEI films,and low electronic and ionic con...A dual-shell Si/TiO2/CFs composite was synthesized through a simple method to deal with the intrinsic drawbacks of silicon-based anode,in terms of huge volume change,unstable SEI films,and low electronic and ionic conductivity.The inner rigid TiO2 shell alleviates the huge volume expansion of the nano silicon,and the outer resilient carbon fiber,which is porous and staggered,is beneficial to the rapid transport of electrons and ions.The as-prepared Si/TiO2/CFs composite displays a superior reversible specific capacity of 583.4 mA·h/g,high rate capability and decent cycling performance.The dual-shell encapsulation method provides a guideline for other anode materials with huge volume expansion during the cycling process.展开更多
In this work, a fast(0.5 h), green microwave-assisted synthesis of single crystalline Sb_2Se_3 nanowires was developed. For the first time we demonstrated a facile solvent-mediated process, whereby intriguing nanostru...In this work, a fast(0.5 h), green microwave-assisted synthesis of single crystalline Sb_2Se_3 nanowires was developed. For the first time we demonstrated a facile solvent-mediated process, whereby intriguing nanostructures including antimony selenide(Sb_2Se_3) nanowires and selenium(Se) microrods can be achieved by merely varying the volume ratio of ethylene glycol(EG) and H_2O free from expensive chemical and additional surfactant. The achieved uniform Sb_2Se_3 nanowire is single crystalline along [001]growth direction with a diameter of 100 nm and a length up to tens of micrometers. When evaluated as an anode of lithium-ion battery, Sb_2Se_3 nanowire can deliver a high reversible capacity of 650.2 m Ah g^(-1) at 100 mA g^(-1) and a capacity retention of 63.8% after long-term 1000 cycles at 1000 mA g^(-1), as well as superior rate capability(389.5 m Ah g^(-1) at 2000 mA g^(-1)). This easy solvent-mediated microwave synthesis approach exhibits its great universe and importance towards the fabrication of high-performance metal chalcogenide electrode materials for future low-cost, large-scale energy storage systems.展开更多
Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy stor...Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy storage systems.Nevertheless,the commercialization of Si-SSBs is significantly impeded by enormous challenges including large volume variation,severe interfacial problems,elusive fundamental mechanisms,and unsatisfied electrochemical performance.Besides,some unknown electrochemical processes in Si-based anode,solid-state electrolytes(SSEs),and Si-based anode/SSE interfaces are still needed to be explored,while an in-depth understanding of solid–solid interfacial chemistry is insufficient in Si-SSBs.This review aims to summarize the current scientific and technological advances and insights into tackling challenges to promote the deployment of Si-SSBs.First,the differences between various conventional liquid electrolyte-dominated Si-based lithium-ion batteries(LIBs)with Si-SSBs are discussed.Subsequently,the interfacial mechanical contact model,chemical reaction properties,and charge transfer kinetics(mechanical–chemical kinetics)between Si-based anode and three different SSEs(inorganic(oxides)SSEs,organic–inorganic composite SSEs,and inorganic(sulfides)SSEs)are systemically reviewed,respectively.Moreover,the progress for promising inorganic(sulfides)SSE-based Si-SSBs on the aspects of electrode constitution,three-dimensional structured electrodes,and external stack pressure is highlighted,respectively.Finally,future research directions and prospects in the development of Si-SSBs are proposed.展开更多
基金Project(51774343) supported by the National Natural Science Foundation of China。
文摘Recycling useful materials such as Ag, Al, Sn, Cu and Si from waste silicon solar cell chips is a sustainable project to slow down the ever-growing amount of waste crystalline-silicon photovoltaic panels. However, the recovery cost of the above-mentioned materials from silicon chips via acid-alkaline treatments outweights the gain economically.Herein, we propose a new proof-of-concept to fabricate Si-based anodes with waste silicon chips as raw materials.Nanoparticles from waste silicon chips were prepared with the high-energy ball milling followed by introducing carbon nanotubes and N-doped carbon into the nanoparticles, which amplifies the electrochemical properties. It is explored that Al and Ag elements influenced electrochemical performance respectively. The results showed that the Al metal in the composite possesses an adverse impact on the electrochemical performance. After removing Al, the composite was confirmed to possess a pronounced durable cycling property due to the presence of Ag, resulting in significantly more superior property than the composite having both Al and Ag removed.
文摘Silicon monoxide(SiO)(silicon[Si]mixed with silicon dioxide[SiO_(2)])/graphite(Gr)composite material is one of the most commercially promising anode materials for the next generation of high-energy-density lithium-ion batteries.The major bottleneck for SiO/Gr composite anode is the poor cyclability arising from the stress/strain behaviors due to the mismatch between two heterogenous materials during the lithiation/delithiation process.To date,a meticulous and quantitative understanding of the highly nonlinear coupling behaviors of such materials is still lacking.Herein,an electro–chemo–mechanics-coupled detailed model containing particle geometries is established.The underlying mechanism of the regulation between SiO and Gr components during electrochemical cycling is quantitatively revealed.We discover that increasing the SiO weight percentage(wt%)reduces the utilization efficiency of the active materials at the same 1C rate charging and enhances the hindering effects of stress-driven flux on diffusion.In addition,the mechanical constraint demonstrates a balanced effect on the overall performance of cells and the local behaviors of particles.This study provides new insights into the fundamental interactions between SiO and Gr materials and advances the investigation methodology for the design and evaluation of next-generation high-energydensity batteries.
基金supported by the National Natural Science Foundation of China(No.62105277)the Natural Science Foundation of Henan Province(No.232300420139)the Internationalization Training of High-Level Talents of Henan Province,and Nanhu Scholars Program for Young Scholars of XYNU.
文摘Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.
基金National Natural Science Foundation of China(No.21905194)Natural Science Foundation of the Jiangsu Higher Education Institution of China(No.23KJB150032).
文摘SiOx is attractive as an anode material for lithium-ion batteries(LIBs)due to its high capacity,low cost,and relatively higher cyclic stability than Si anode.However,the intrinsic low electronic conductivity,low initial coulombic efficiency(ICE),and volume expansion during cycles hinder its applications.In this review,we summarize advances in high performance SiOx anodes,mainly from two aspects:active material and binders.The future perspective is investigated at the end of this review.Our review provides strategical guidance for developing high performance SiOx anodes.
基金supported by Shaanxi Yanchang Petroleum Co.,Ltd.(18529)Yiwu Research Institute of Fudan University(21557)+1 种基金the National Science Foundation of China(22075048)the Shanghai International Collaboration Research Project(19520713900).
文摘Implementing high-performance silicon(Si)anode in actual processing and application is highly desirable for next-generation,high-energy Li-ion batteries.However,high content of inactive matrix(including conductive agent and binder)is often indispensable in order to ensure local conductivity and suppress pulverization tendency of Si particles,which thus cause great capacity loss based on the mass of whole electrode.Here,we designed an accordion-structured,high-performance electrode with high Si content up to 95%.Si nanoparticles were well anchored into the interlayer spacings of accordion-like graphene arrays,and free-standing electrode was prepared via a simple filtration process without any binder.Conductive accordion framework ensures strong confinement effect of Si nanoparticles and also provides direct,non-tortuous channels for fast electrochemical reaction kinetics.As a consequence,the accordion Si electrodes exhibit ultrahigh,electrode-based capacities up to 3149 mAh g^(-1)(under Si content of 91%),as well as long-term stability.Also,the accordion electrode can bear extreme condition of over-lithiation and maintains stable in full-cell test.This design provides a significant stride in high Si content toward realistic,high-performance electrodes.
基金supported by the Fundamental Research Funds for Central Universities of China and the Key Research and Development Projects of Sichuan(No.2020YFG0127)。
文摘Low-cost silicon microparticles(SiMP),as a substitute for nanostructured silicon,easily suffer from cracks and fractured during the electrochemical cycle.A novel n-type conductive polymer binder with excellent electronic and ionic conductivities as well as good adhesion,has been successfully designed and applied for high-performance SiMP anodes in lithium-ion batteries to address this problem.Its unique features are attributed to the stro ng electron-withdrawing oxadiazole ring structure with sulfonate polar groups.The combination of rigid and flexible components in the polymer ensures its good mechanical strength and ductility,which is beneficial to suppress the expansion and contraction of SiMP s during the charge/discharge process.By fine-tuning the monomer ratio,the conjugation and sulfonation degrees of the polymer can be precisely controlled to regulate its ionic and electronic conductivities,which has been systematically analyzed with the help of an electrochemical test method,filling in the gap on the conductivity measurement of the polymer in the doping state.The experimental results indicate that the cell with the developed n-type polymer binder and SiMP(~0.5 μm) anodes achieves much better cycling performance than traditional non-conductive binders.It has been considered that the initial capacity of the SiMP anode is controlled by the synergetic effect of ionic and electronic conductivity of the binder,and the capacity retention mainly depends on its electronic conductivity when the ionic conductivity is sufficient.It is worth noting that the fundamental research of this wo rk is also applicable to other battery systems using conductive polymers in order to achieve high energy density,broadening their practical applications.
基金Project(51772331)supported by the National Natural Science Foundation of ChinaProject(2018YFB1106000)supported by the National Key Technologies R&D Program of China
文摘A dual-shell Si/TiO2/CFs composite was synthesized through a simple method to deal with the intrinsic drawbacks of silicon-based anode,in terms of huge volume change,unstable SEI films,and low electronic and ionic conductivity.The inner rigid TiO2 shell alleviates the huge volume expansion of the nano silicon,and the outer resilient carbon fiber,which is porous and staggered,is beneficial to the rapid transport of electrons and ions.The as-prepared Si/TiO2/CFs composite displays a superior reversible specific capacity of 583.4 mA·h/g,high rate capability and decent cycling performance.The dual-shell encapsulation method provides a guideline for other anode materials with huge volume expansion during the cycling process.
基金supported by the National Key Research and Development Program of China(2016YFA0202603)the National Basic Research Program of China(2013CB934103)+5 种基金the National Natural Science Foundation of China(51521001,51602239)the National Natural Science Fund for Distinguished Young Scholars(51425204)Yellow Crane Talent(Science&Technology)Program of Wuhan Citythe Fundamental Research Funds for the Central Universities(WUT:2016III001,2016III003,2016IVA090)the Programme of Introducing Talents of Discipline to Universities(B17034)support from the Lorraine Region(nowpart of Grand Est Region)Cooperation Research Lorraine/Hubei Program 2015/2017
文摘In this work, a fast(0.5 h), green microwave-assisted synthesis of single crystalline Sb_2Se_3 nanowires was developed. For the first time we demonstrated a facile solvent-mediated process, whereby intriguing nanostructures including antimony selenide(Sb_2Se_3) nanowires and selenium(Se) microrods can be achieved by merely varying the volume ratio of ethylene glycol(EG) and H_2O free from expensive chemical and additional surfactant. The achieved uniform Sb_2Se_3 nanowire is single crystalline along [001]growth direction with a diameter of 100 nm and a length up to tens of micrometers. When evaluated as an anode of lithium-ion battery, Sb_2Se_3 nanowire can deliver a high reversible capacity of 650.2 m Ah g^(-1) at 100 mA g^(-1) and a capacity retention of 63.8% after long-term 1000 cycles at 1000 mA g^(-1), as well as superior rate capability(389.5 m Ah g^(-1) at 2000 mA g^(-1)). This easy solvent-mediated microwave synthesis approach exhibits its great universe and importance towards the fabrication of high-performance metal chalcogenide electrode materials for future low-cost, large-scale energy storage systems.
基金supported by the National Natural Science Foundation of China(Grants Nos.52072323,52122211 and 21875155)the State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(Grant No.LAPS22005)+3 种基金the Frontier Exploration Projects of Longmen Laboratory(Grant No.LMQYTSKT008)the Shenzhen Technical Plan Project(No.JCYJ20220818101003008)the support of High-Tech Industrialization Project of Tan Kah Kee Innovation Laboratory(Grant No.RD2021010101)the“Double-First Class”Foundation of Materials and Intelligent Manufacturing Discipline of Xiamen University.L.Zhang and Q.Zhang acknowledge the support of the Nanqiang Young Top-notch Talent Fellowship at Xiamen University.
文摘Silicon(Si)-based solid-state batteries(Si-SSBs)are attracting tremendous attention because of their high energy density and unprecedented safety,making them become promising candidates for next-generation energy storage systems.Nevertheless,the commercialization of Si-SSBs is significantly impeded by enormous challenges including large volume variation,severe interfacial problems,elusive fundamental mechanisms,and unsatisfied electrochemical performance.Besides,some unknown electrochemical processes in Si-based anode,solid-state electrolytes(SSEs),and Si-based anode/SSE interfaces are still needed to be explored,while an in-depth understanding of solid–solid interfacial chemistry is insufficient in Si-SSBs.This review aims to summarize the current scientific and technological advances and insights into tackling challenges to promote the deployment of Si-SSBs.First,the differences between various conventional liquid electrolyte-dominated Si-based lithium-ion batteries(LIBs)with Si-SSBs are discussed.Subsequently,the interfacial mechanical contact model,chemical reaction properties,and charge transfer kinetics(mechanical–chemical kinetics)between Si-based anode and three different SSEs(inorganic(oxides)SSEs,organic–inorganic composite SSEs,and inorganic(sulfides)SSEs)are systemically reviewed,respectively.Moreover,the progress for promising inorganic(sulfides)SSE-based Si-SSBs on the aspects of electrode constitution,three-dimensional structured electrodes,and external stack pressure is highlighted,respectively.Finally,future research directions and prospects in the development of Si-SSBs are proposed.