The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration ...The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.展开更多
Layered Ni-rich cathode materials,LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622),are synthesized via solid reaction assisted with a plasma milling pretreatment,which is resulted in lowering sintering temperatures for solid p...Layered Ni-rich cathode materials,LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622),are synthesized via solid reaction assisted with a plasma milling pretreatment,which is resulted in lowering sintering temperatures for solid precursors.The plasma milling pretreated NCM622 cathode material sintered at 780℃(named as PM-780)demonstrates good cycling stability at both room and subzero temperatures.Specifically,the PM-780 cathode delivers an initial discharge capacity of 171.2 mAh g^(-1) and a high capacity retention of 99.7%after 300 cycles with current rate of 90 mA g^(-1) at 30℃,while stable capacities of 120.3 and 94.0 m Ah g^(-1) can be remained at-10℃and-20℃in propylene carbonate contained electrolyte,respectively.In-situ XRD together with XPS and SEM reveal that the NCM622 cycled at-10℃presented better structural stability and more intact interface than that of cathodes cycled at 30℃.It is also found that subzero temperatures only limit the discharge potential of NCM622 without destroying its structure during cycling since it still exhibits high discharge capacity at 30℃after cycled at subzero temperatures.This work may expand the knowledge about the low-temperature characteristics of layered cathode materials for Li-ion batteries and lay the foundation for its further applications.展开更多
In the past two decades,a lot of high-capacity conversion-type metal oxides have been intensively studied as alternative anode materials for Li-ion batteries with higher energy density.Unfortunately,their large voltag...In the past two decades,a lot of high-capacity conversion-type metal oxides have been intensively studied as alternative anode materials for Li-ion batteries with higher energy density.Unfortunately,their large voltage hysteresis(0.8-1.2 V) within reversed conversion reactions results in huge round-trip inefficiencies and thus lower energy efficiency(50%-75%) in full cells than those with graphite anodes.This remains a long-term open question and has been the most serious drawback toward application of metal oxide anodes.Here we clarify the origins of voltage hysteresis in the typical SnO2anode and propose a universal strategy to minimize it.With the established in situ phosphating to generate metal phosphates during reversed conversion reactions in synergy with boosted reaction kinetics by the added P and Mo,the huge voltage hysteresis of 0.9 V in SnO_(2),SnO_(2)-Mo,and 0.6 V in SnO2-P anodes is minimized to 0.3 V in a ternary SnO_(2)-Mo-P(SOMP) composite,along with stable high capacity of 936 mA h g^(-1)after 800 cycles.The small voltage hysteresis can remain stable even the SOMP anode operated at high current rate of10 A g^(-1)and wide-range temperatures from 60 to 30℃,resulting in a high energy efficiency of88.5% in full cells.This effective strategy to minimize voltage hysteresis has also been demonstrated in Fe2O3,Co3O4-basded conversion-type anodes.This work provides important guidance to advance the high-capacity metal oxide anodes from laboratory to industrialization.展开更多
Silicon monoxide(SiO)has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries.To enhance the initial Coulombic efficiencies(ICE)and cycle stability of SiO-based anod...Silicon monoxide(SiO)has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries.To enhance the initial Coulombic efficiencies(ICE)and cycle stability of SiO-based anodes,a new facile composition and electrode design strategy have been adapted to fabricate a SiO-Sn-Co/graphite(G)anode.It achieves a unique structure where tiny milled SiO-Sn-Co particles are dispersed among two graphite layers.In this hybrid electrode,Sn-Co alloys promoted Li;extraction kinetics,and the holistic reversibility of SiO and graphite enhanced the electrical conductivity.The SiO-Sn-Co/G electrode delivered an average ICE of 77.6%and a reversible capacity of 640 mAh g^(-1)at 800 mA g^(-1),and the capacity retention was above 98%after 100 cycles,which was much higher than that of the SiO with an ICE of 55.3%and a capacity retention of 50%.These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO anode.Furthermore,based on its easy and feasible fabrication process,it may provide a suitable choice to combine other alloy anodes with the graphite anode.展开更多
Transition metal nitrides are highly valued owing to their unique properties and diverse applications in coatings,lighting applications,and energy storage.However,the development two-dimensional(2D)metal nitrides pres...Transition metal nitrides are highly valued owing to their unique properties and diverse applications in coatings,lighting applications,and energy storage.However,the development two-dimensional(2D)metal nitrides presents a significant challenge owing to their strong atomic bonds.Herein,we introduce a family of 2D multicomponent metal nitrides,metal tungsten nitride(MWN_(2))nanosheets,via a precursor minimization and nitridation strategy.The composition of M and the stoichiometric ratio can be readily tailored,enabling the successful preparation of high-entropy(FeCoNiMn)WN_(2)nanosheets.Prominently,the high-entropy MWN_(2)nanosheets demonstrate superior oxygen evolution with an overpotential of only 228 mV at 10 mA cm^(−2)and exceptional stability,exhibiting a degradation rate of merely 15μV h^(−1)over 1000 hours.Theoretical insights reveal that antisite defects substantially lower the oxygen adsorption energy.This work sheds light on the highly active and stable catalytic properties of 2D metal nitrides for water oxidation.展开更多
The unstable interfaces between a SnO_(2)anode and an electrolyte in a Li-ion battery dramatically impair the reversibility and cycling stability of lithiation and delithiation,resulting in low roundtrip Coulombic eff...The unstable interfaces between a SnO_(2)anode and an electrolyte in a Li-ion battery dramatically impair the reversibility and cycling stability of lithiation and delithiation,resulting in low roundtrip Coulombic efficiency(CE)and fast capacity decay of SnO_(2)-based anode materials.Herein,a simple strategy of modifying the solid electrolyte interphase(SEI)is developed to enhance the interfacial stability and lithium storage reversibility of SnO_(2)by compositing it with graphite(G)and an inorganic component of the SEI,such as Li_(2)CO_(3)or LiF,which results in the SnO_(2)-Li_(2)CO_(3)/G and SnO_(2)-LiF/G composite anodes with high CEs,large capacities and long cycle lives.Specifically,the SnO_(2)-Li_(2)CO_(3)/G composite anode exhibits an average initial CE of 79.6%,a stable reversible capacity of 927.5 mA hg^(-1)at a current rate of 0.2 A g^(-1),and a charge capacity over 1200 mA hg^(-1)with a CE>99%after 900 cycles at a higher current rate of 1 A g^(-1).It is revealed that Li_(2)CO_(3)induces the formation of a dense and stable SEI on SnO_(2)grains and inhibits the coarsening of nanosized Sn particles generated from the dealloying reaction in the SnO_(2)-Li_(2)CO_(3)/G electrode.Moreover,the CE and cycling stability of other alloying-type(Si)and conversion reaction(MnO_(2)and Fe_(3)O_(4))anodes can also be greatly promoted by simply milling with Li_(2)CO_(3).Thus,a universal and simple strategy is developed to achieve highly reversible and stable electrodes for large-capacity lithium storage.展开更多
基金financial support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52372250,52125105,52173242)+1 种基金Shenzhen Science and Technology Planning Project(RCYX20221008092850072,JSGG20220831104004008,KJZD20230923113859006,JCYJ20220531100405012,KJZD20241122161900001)Science and Technology Planning Project of Guangdong Province(2024A1515030076)。
文摘The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.
基金supported by the National Natural Science Foundation of China(No.51671088,51621001,51822104 and 51831009)the Guangzhou Science and Technology Plan Projects(No.201904020018)the Fundamental Research Funds for the Central Universities in South China University of Technology(No.2019CG24)。
文摘Layered Ni-rich cathode materials,LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622),are synthesized via solid reaction assisted with a plasma milling pretreatment,which is resulted in lowering sintering temperatures for solid precursors.The plasma milling pretreated NCM622 cathode material sintered at 780℃(named as PM-780)demonstrates good cycling stability at both room and subzero temperatures.Specifically,the PM-780 cathode delivers an initial discharge capacity of 171.2 mAh g^(-1) and a high capacity retention of 99.7%after 300 cycles with current rate of 90 mA g^(-1) at 30℃,while stable capacities of 120.3 and 94.0 m Ah g^(-1) can be remained at-10℃and-20℃in propylene carbonate contained electrolyte,respectively.In-situ XRD together with XPS and SEM reveal that the NCM622 cycled at-10℃presented better structural stability and more intact interface than that of cathodes cycled at 30℃.It is also found that subzero temperatures only limit the discharge potential of NCM622 without destroying its structure during cycling since it still exhibits high discharge capacity at 30℃after cycled at subzero temperatures.This work may expand the knowledge about the low-temperature characteristics of layered cathode materials for Li-ion batteries and lay the foundation for its further applications.
基金financially supported by the National Natural Science Foundation of China (Nos. 52071144, 52231009,51831009, 51901043)the Guangdong Basic and Applied Basic Research Foundation (No. 2023B1515040011)+1 种基金the Guangzhou Key Research and Development Program (No. 202103040001)the TCL Science and Technology Innovation Fund (No.20222055)。
文摘In the past two decades,a lot of high-capacity conversion-type metal oxides have been intensively studied as alternative anode materials for Li-ion batteries with higher energy density.Unfortunately,their large voltage hysteresis(0.8-1.2 V) within reversed conversion reactions results in huge round-trip inefficiencies and thus lower energy efficiency(50%-75%) in full cells than those with graphite anodes.This remains a long-term open question and has been the most serious drawback toward application of metal oxide anodes.Here we clarify the origins of voltage hysteresis in the typical SnO2anode and propose a universal strategy to minimize it.With the established in situ phosphating to generate metal phosphates during reversed conversion reactions in synergy with boosted reaction kinetics by the added P and Mo,the huge voltage hysteresis of 0.9 V in SnO_(2),SnO_(2)-Mo,and 0.6 V in SnO2-P anodes is minimized to 0.3 V in a ternary SnO_(2)-Mo-P(SOMP) composite,along with stable high capacity of 936 mA h g^(-1)after 800 cycles.The small voltage hysteresis can remain stable even the SOMP anode operated at high current rate of10 A g^(-1)and wide-range temperatures from 60 to 30℃,resulting in a high energy efficiency of88.5% in full cells.This effective strategy to minimize voltage hysteresis has also been demonstrated in Fe2O3,Co3O4-basded conversion-type anodes.This work provides important guidance to advance the high-capacity metal oxide anodes from laboratory to industrialization.
基金supported by the National Natural Science Foundation of China (No. 52071144, 51822104, 51831009, and 51621001)
文摘Silicon monoxide(SiO)has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries.To enhance the initial Coulombic efficiencies(ICE)and cycle stability of SiO-based anodes,a new facile composition and electrode design strategy have been adapted to fabricate a SiO-Sn-Co/graphite(G)anode.It achieves a unique structure where tiny milled SiO-Sn-Co particles are dispersed among two graphite layers.In this hybrid electrode,Sn-Co alloys promoted Li;extraction kinetics,and the holistic reversibility of SiO and graphite enhanced the electrical conductivity.The SiO-Sn-Co/G electrode delivered an average ICE of 77.6%and a reversible capacity of 640 mAh g^(-1)at 800 mA g^(-1),and the capacity retention was above 98%after 100 cycles,which was much higher than that of the SiO with an ICE of 55.3%and a capacity retention of 50%.These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO anode.Furthermore,based on its easy and feasible fabrication process,it may provide a suitable choice to combine other alloy anodes with the graphite anode.
基金financially supported by the National Natural Science Foundation of China(No.22275205,22205148,and 52403381)the Science and Technology Foundation of Shenzhen(No.JCYJ20220530154404010,JCYJ20230807140900001,and JCYJ20220818100806014)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(No.2023B1515020102 and 2022A1515110408)supported by the public computing service platform provided by SIAT.
文摘Transition metal nitrides are highly valued owing to their unique properties and diverse applications in coatings,lighting applications,and energy storage.However,the development two-dimensional(2D)metal nitrides presents a significant challenge owing to their strong atomic bonds.Herein,we introduce a family of 2D multicomponent metal nitrides,metal tungsten nitride(MWN_(2))nanosheets,via a precursor minimization and nitridation strategy.The composition of M and the stoichiometric ratio can be readily tailored,enabling the successful preparation of high-entropy(FeCoNiMn)WN_(2)nanosheets.Prominently,the high-entropy MWN_(2)nanosheets demonstrate superior oxygen evolution with an overpotential of only 228 mV at 10 mA cm^(−2)and exceptional stability,exhibiting a degradation rate of merely 15μV h^(−1)over 1000 hours.Theoretical insights reveal that antisite defects substantially lower the oxygen adsorption energy.This work sheds light on the highly active and stable catalytic properties of 2D metal nitrides for water oxidation.
基金the National Natural Science Foundation of China(52071144,51621001,51822104 and 51831009)。
文摘The unstable interfaces between a SnO_(2)anode and an electrolyte in a Li-ion battery dramatically impair the reversibility and cycling stability of lithiation and delithiation,resulting in low roundtrip Coulombic efficiency(CE)and fast capacity decay of SnO_(2)-based anode materials.Herein,a simple strategy of modifying the solid electrolyte interphase(SEI)is developed to enhance the interfacial stability and lithium storage reversibility of SnO_(2)by compositing it with graphite(G)and an inorganic component of the SEI,such as Li_(2)CO_(3)or LiF,which results in the SnO_(2)-Li_(2)CO_(3)/G and SnO_(2)-LiF/G composite anodes with high CEs,large capacities and long cycle lives.Specifically,the SnO_(2)-Li_(2)CO_(3)/G composite anode exhibits an average initial CE of 79.6%,a stable reversible capacity of 927.5 mA hg^(-1)at a current rate of 0.2 A g^(-1),and a charge capacity over 1200 mA hg^(-1)with a CE>99%after 900 cycles at a higher current rate of 1 A g^(-1).It is revealed that Li_(2)CO_(3)induces the formation of a dense and stable SEI on SnO_(2)grains and inhibits the coarsening of nanosized Sn particles generated from the dealloying reaction in the SnO_(2)-Li_(2)CO_(3)/G electrode.Moreover,the CE and cycling stability of other alloying-type(Si)and conversion reaction(MnO_(2)and Fe_(3)O_(4))anodes can also be greatly promoted by simply milling with Li_(2)CO_(3).Thus,a universal and simple strategy is developed to achieve highly reversible and stable electrodes for large-capacity lithium storage.
