Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.I...Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.展开更多
Although lithium-ion batteries are widely recognized as a new generation of energy storage devices,their large-scale application is severely hampered by their low energy density and restricted cyclic stability.Herein,...Although lithium-ion batteries are widely recognized as a new generation of energy storage devices,their large-scale application is severely hampered by their low energy density and restricted cyclic stability.Herein,an ingenious dual-modified interface,where the F-doping and fluorocarbon coating co-existed on Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)surface,is rationally constructed to elevate its energy density and structural stability attributed to F-grafting between the bulk material and the coating utilizing a robust super-conformal fluorocarbon coating structural framework and more stable F-doped system under high charge/discharge cut-off voltage.In comparison with a single carbon-coated modified Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2),the dual-modified sample overcomes the fatal disadvantage of carbon coating stripping during long-period cycles ascribed to the“TM-F-multifunctional coating”connector which firmly combines the bulk material with the coating with a strong interaction force,exhibiting a more stable-reversible structure and excellent comprehensive electrochemical performance under high cut-off voltage.Concomitantly,the F-transition metal bonds with stronger bond energies improve its structural reversibility during the processes of charge/discharge under high voltage.Furthermore,the fluorocarbon coating enhances its charge transfer ability and effectively restrains the interfacial side reactions.Additionally,the climbing nudged elastic band methodology is used to calculate the diffusion energy barrier of lithium-ions in the matrix material,which confirms the fundamental reason for its superior lithium-ion diffusion ability.The high pseudocapacitance contribution ratio is perfectly explained by calculating the adsorption capacity on the surface of the dual-modified sample.Consequently,experiments and theoretical calculations unequivocally confirm its distinguished electrochemical properties under high cut-off voltage.展开更多
LiNi0.8Co0.1Mn0.1O2(NCM811)|SiOx-graphite(SiO-Gr.)battery chemistry is of intensive attention because its achievable practical energy density is approaching impressively 300 Wh Kg^(-1).However,it still suffers rapid c...LiNi0.8Co0.1Mn0.1O2(NCM811)|SiOx-graphite(SiO-Gr.)battery chemistry is of intensive attention because its achievable practical energy density is approaching impressively 300 Wh Kg^(-1).However,it still suffers rapid capacity fades during repeated cycles,both chemical,electrochemical and mechanical irreversibility contribute.A comprehensive understanding behind the fading behavior of the cell chemistry is required before fully realize the benefits of this chemistry.Herein,the in-situ thickness variation is introduced as a diagnostic technique and is performed on 5-55 Ah NCM811|SiO-Gr cells.With the help of Li reference electrode and in-situ X-ray diffraction device,the correspondence between thickness variation and the electrode potential is carefully investigated.Firstly,the NCM811|SiO-Gr cell is characterized with the maximum cell thickness at around 80%state-of-charge(SOC)in the discharge process,rather than at 100%SOC.Secondly,the electrochemical behaviors during rate charge/discharge are diagnosed,and a Li platting signal is resolved from thickness variation profile at 2C.This work confirms that the thickness monitoring is a nondestructive and informative complement to conventional diagnostic techniques for failure analysis of pouch cells.展开更多
High-performance thick electrodes are regarded as a feasible strategy for enhancing the energy density of lithium-ion batteries.However,fast ion transport and long-life cyclability in thick cathode remain significant ...High-performance thick electrodes are regarded as a feasible strategy for enhancing the energy density of lithium-ion batteries.However,fast ion transport and long-life cyclability in thick cathode remain significant challenges.Here,we developed a multidirectional-ion-transport Ni-rich thick cathode LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),which exhibits excellent consecutive layer-by-layer contact and fast ion-flow diffusion,achieving high areal capacity and superior rate capability toward 3D-printed batteries.By balancing the viscosity of electrode inks and mechanical strength of thick electrodes,a multilayer NCM811 cathode with strong interfacial bonding,reaching an electrode thickness of 3 mm and ultra-high mass loading of 185 mg cm^(-2),delivers a record areal capacity of 38.4 mAh cm^(-2)up to date.The 3D-printed porous frameworks featuring the multidirectional transport of Li ion and superior affinity of electrolyte,exceptionally boost active material utilization and fast electrochemical kinetics of thick electrodes,resulting in a high specific capacity of 208 mAh g^(-1).Furthermore,the printed electrode has a capacity retention rate of 88%after 150 cycles at 2 C.A full cell assembled with a printed NCM811 cathode and graphite anode shows high energy density of 417 Wh kg^(-1)at electrode level and long-term cyclability.This work provides an effective strategy for fabricating long-lifespan and high-energy-density lithium-ion batteries.展开更多
LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)material,as the promising cathode candidate for next-generation highenergy lithium-ion batteries,has gained considerable attention for extremely high theoretical capacity and low...LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)material,as the promising cathode candidate for next-generation highenergy lithium-ion batteries,has gained considerable attention for extremely high theoretical capacity and low cost.Nevertheless,the intrinsic drawbacks of NCM811 such as unstable structure and inevitable interface side reaction result in severe capacity decay and thermal runaway.Herein,a novel polyimide(denoted as PI-Om DT)constructed with the highly polar and micro-branched crosslinking network is reported as a binder material for NCM811 cathode.The micro-branched crosslinking network is achieved by using 1,3,5-Tris(4-aminophenoxy)benzene(TAPOB)as a crosslinker via condensation reaction,which endows excellent mechanical properties and large free volume.Meanwhile,the massive polar carboxyl(-COOH)groups provide strong adhesion sites to active NCM811 particles.These functions of PIOm DT binder collaboratively benefit to forming the mechanically robust and homogeneous coating layer with rapid Li+diffusion on the surface of NCM811,significantly stabilizing the cathode structure,suppressing the detrimental interface side reaction and guaranteeing the shorter ion-diffusion and electron-transfer paths,consequently enhancing electrochemical performance.As compared to the NCM811 with PVDF binder,the NCM811 using PI-Om DT binder delivers a superior high-rate capacity(121.07 vs.145.38 m Ah g^(-1))at 5 C rate and maintains a higher capacity retention(80.38%vs.91.6%)after100 cycles at 2.5–4.3 V.Particularly,at the high-voltage conditions up to 4.5 and 4.7 V,the NCM811 with PI-Om DT binder still maintains the remarkable capacity retention of 88.86%and 72.5%after 100 cycles,respectively,paving the way for addressing the high-voltage operating stability of the NCM811 cathode.Moreover,the full-charged NCM811 cathode with PI-Om DT binder exhibits a significantly enhanced thermal stability,improving the safety performance of batteries.This work opens a new avenue for developing high-energy NCM811 based lithium-ion batteries with long cycle-life and superior safety performance using a novel and effective binder.展开更多
With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control...With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control synthesis routes based on repetitive experiments are often costly and inefficient,which is unsuitable for the broader application of novel materials.The development of machine learning and its combination with materials design offers a potential pathway for optimizing materials.Here,we present a design synthesis paradigm for developing high energy Ni-rich cathodes with thermal/kinetic simulation and propose a coupled image-morphology machine learning model.The paradigm can accurately predict the reaction conditions required for synthesizing cathode precursors with specific morphologies,helping to shorten the experimental duration and costs.After the model-guided design synthesis,cathode materials with different morphological characteristics can be obtained,and the best shows a high discharge capacity of 206 mAh g^(−1)at 0.1C and 83%capacity retention after 200 cycles.This work provides guidance for designing cathode materials for lithium-ion batteries,which may point the way to a fast and cost-effective direction for controlling the morphology of all types of particles.展开更多
LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),a high-nickel layered oxide,has emerged as a frontrunner for next-generation lithium-ion batteries(LIBs)due to its high energy density,excellent rate performance,and cost-effect...LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),a high-nickel layered oxide,has emerged as a frontrunner for next-generation lithium-ion batteries(LIBs)due to its high energy density,excellent rate performance,and cost-effectiveness.However,NCM811 cathodes face multifaceted challenges,including cation mixing,microcracking,and residual lithium compounds,necessitating a comprehensive understanding for addressing these critical issues.In this review,we provide an in-depth analysis of recent advancements,presenting actionable insights into effective strategies to address the key issues in the NCM811 cathode and proposing pathways for optimizing NCM811 cathodes in LIB applications.Additionally,the forward-looking perspectives are explored in this review,highlighting the role of advanced material characterization techniques,theoretical modeling,and computational simulations in overcoming the inherent limitations of NCM811 cathodes.By synthesizing current knowledge and technological advancements,this review aims to serve as a foundational resource for researchers and industry professionals striving to enhance the performance and accelerate the commercialization of NCM811 cathode materials,contributing to the future of energy storage solutions.展开更多
At present,lithium-ion batteries(LIBs)have been vastly applied and are widely being used for portable device,hybrid electric vehicles,and aviation field.Cathode materials,as the most important part in the LIBs,shows a...At present,lithium-ion batteries(LIBs)have been vastly applied and are widely being used for portable device,hybrid electric vehicles,and aviation field.Cathode materials,as the most important part in the LIBs,shows a profound prospect and potential.This study mainly focuses on the study of the means of how to improve the electrochemical properties and performance of the NCM cathode materials,examining the characterization of the NCM cathode materials through the characterization techniques.By referring different doping elements on NCM cathode materials,this paper aims to examine the structural properties,electrochemical performance,and stability of these materials under different dopants.Several characterization techniques,inductively coupled plasma(ICP),x-ray photoelectron spectroscope(XPS),Scanning electron microscopy(SEM),transmission electron microscopy(TEM),energy dispersive spectroscope(EDS),and x-ray diffraction(XRD)results have clearly displayed a large amount of figure on cathode materials,which help us to gain a better understanding on the characteristic of each cathode materials and help us to do the further calculation and study on cathode materials.展开更多
Solid-state batteries(SSBs)are a promising next step in electrochemical energy storage but are plagued by a number of problems.In this study,we demonstrate the recurring issue of mechanical degradation because of volu...Solid-state batteries(SSBs)are a promising next step in electrochemical energy storage but are plagued by a number of problems.In this study,we demonstrate the recurring issue of mechanical degradation because of volume changes in layered Ni-rich oxide cathode materials in thiophosphate-based SSBs.Specifically,we explore superionic solid electrolytes(SEs)of different crystallinity,namely glassy 1.5Li_(2)S-0.5P_(2)S_(5)-LiI and argyrodite Li_(6)PS_(5)Cl,with emphasis on how they affect the cyclability of slurry-cast cathodes with NCM622(60%Ni)or NCM851005(85%Ni).The application of a combination of ex situ and in situ analytical techniques helped to reveal the benefits of using a SE with a low Young’s modulus.Through a synergistic interplay of(electro)chemical and(chemo)mechanical effects,the glassy SE employed in this work was able to achieve robust and stable interfaces,enabling intimate contact with the cathode material while at the same time mitigating volume changes.Our results emphasize the importance of considering chemical,electrochemical,and mechanical properties to realize long-term cycling performance in high-loading SSBs.展开更多
Promoting industry applications of high-energy Li metal batteries(LMBs)is of vital importance for accelerating the electrification and decarbonization of our society.Unfortunately,the time-dependent storage aging of A...Promoting industry applications of high-energy Li metal batteries(LMBs)is of vital importance for accelerating the electrification and decarbonization of our society.Unfortunately,the time-dependent storage aging of Ah-level Li metal pouch cells,a ubiquitous but crucial practical indicator,has not yet been revealed.Herein,we first report the storage behaviors and multilateral synergistic aging mechanism of Ah-level NCM811jjLi pouch cells during the 120-day long-term storage under various conditions.Contrary to the conventional belief of Li-ion batteries with graphite intercalation anodes,the significant available capacity loss of 32.8%on average originates from the major electrolyte-sensitive anode corrosion and partial superimposed cathode degradation,and the irreversible capacity loss of 13.3%is essentially attributed to the unrecoverable interface/structure deterioration of NCM with further hindrance of the aged Li.Moreover,principles of alleviating aging have been proposed.This work bridges academia and industry and enriches the fundamental epistemology of storage aging of LMBs,shedding light on realistic applications of high-energy batteries.展开更多
基金supported by the Australian Research Council via Discovery Projects(Nos.DP200103315,DP200103332 and DP230100685)Linkage Projects(No.LP220200920)+1 种基金support from the IONTOF M6 ToF-SIMS(funded by ARC LIEF,LE190100053)the Kratos Axis Ultra XPS(ARC LIEF,LE120100026)。
文摘Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.
基金support from the Natural Science Foundation of Fujian Province,China(No.2021H0028)the Natural Science Foundation of China(No.21975212)+1 种基金Open Fund of Fujian Provincial Key Laboratory of Functional Materials and Applications(No.fma2023003)the Science and Technology Planning Project of Xiamen City(No.2022CXY0409).
文摘Although lithium-ion batteries are widely recognized as a new generation of energy storage devices,their large-scale application is severely hampered by their low energy density and restricted cyclic stability.Herein,an ingenious dual-modified interface,where the F-doping and fluorocarbon coating co-existed on Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2)surface,is rationally constructed to elevate its energy density and structural stability attributed to F-grafting between the bulk material and the coating utilizing a robust super-conformal fluorocarbon coating structural framework and more stable F-doped system under high charge/discharge cut-off voltage.In comparison with a single carbon-coated modified Li[Ni_(0.8)Co_(0.1)Mn_(0.1)]O_(2),the dual-modified sample overcomes the fatal disadvantage of carbon coating stripping during long-period cycles ascribed to the“TM-F-multifunctional coating”connector which firmly combines the bulk material with the coating with a strong interaction force,exhibiting a more stable-reversible structure and excellent comprehensive electrochemical performance under high cut-off voltage.Concomitantly,the F-transition metal bonds with stronger bond energies improve its structural reversibility during the processes of charge/discharge under high voltage.Furthermore,the fluorocarbon coating enhances its charge transfer ability and effectively restrains the interfacial side reactions.Additionally,the climbing nudged elastic band methodology is used to calculate the diffusion energy barrier of lithium-ions in the matrix material,which confirms the fundamental reason for its superior lithium-ion diffusion ability.The high pseudocapacitance contribution ratio is perfectly explained by calculating the adsorption capacity on the surface of the dual-modified sample.Consequently,experiments and theoretical calculations unequivocally confirm its distinguished electrochemical properties under high cut-off voltage.
基金funded by the Ministry of Science and Technology of China(No.2019YFE0100200,2019YFA0705703)the National Natural Science Foundation of China(No.22075064,No.21875057,U1564205 and 51706117)+1 种基金the Key-Area Research and Development Program of Guangdong Province(No.2020B090919005)the Tsinghua University Initiative Scientific Research Program(No.2019Z02UTY06).
文摘LiNi0.8Co0.1Mn0.1O2(NCM811)|SiOx-graphite(SiO-Gr.)battery chemistry is of intensive attention because its achievable practical energy density is approaching impressively 300 Wh Kg^(-1).However,it still suffers rapid capacity fades during repeated cycles,both chemical,electrochemical and mechanical irreversibility contribute.A comprehensive understanding behind the fading behavior of the cell chemistry is required before fully realize the benefits of this chemistry.Herein,the in-situ thickness variation is introduced as a diagnostic technique and is performed on 5-55 Ah NCM811|SiO-Gr cells.With the help of Li reference electrode and in-situ X-ray diffraction device,the correspondence between thickness variation and the electrode potential is carefully investigated.Firstly,the NCM811|SiO-Gr cell is characterized with the maximum cell thickness at around 80%state-of-charge(SOC)in the discharge process,rather than at 100%SOC.Secondly,the electrochemical behaviors during rate charge/discharge are diagnosed,and a Li platting signal is resolved from thickness variation profile at 2C.This work confirms that the thickness monitoring is a nondestructive and informative complement to conventional diagnostic techniques for failure analysis of pouch cells.
基金supported by the National Natural Science Foundation of China(22125903,22439003,22479128,22209175,22309176,22209173)the National Key R&D Program of China(2022YFA1504100)+6 种基金the Liaoning Revitalization Talents Program-Leading Talents(XLYC2402032)the United Foundation for Dalian Institute of Chemical Physics,Chinese Academy of Sciences and Shenyang Institute of Automation,Chinese Academy of Sciences(DICP&SIA UN202501)the State Key Laboratory of Catalysis(2024SKL-A-001)the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(E412010508)the S&T Program of Energy Shaanxi Laboratory(ESL B202403)the Natural Science Foundation of Liaoning Province(2023BS006)the China National Postdoctoral Program for Innovative Talents(BX20240334)。
文摘High-performance thick electrodes are regarded as a feasible strategy for enhancing the energy density of lithium-ion batteries.However,fast ion transport and long-life cyclability in thick cathode remain significant challenges.Here,we developed a multidirectional-ion-transport Ni-rich thick cathode LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),which exhibits excellent consecutive layer-by-layer contact and fast ion-flow diffusion,achieving high areal capacity and superior rate capability toward 3D-printed batteries.By balancing the viscosity of electrode inks and mechanical strength of thick electrodes,a multilayer NCM811 cathode with strong interfacial bonding,reaching an electrode thickness of 3 mm and ultra-high mass loading of 185 mg cm^(-2),delivers a record areal capacity of 38.4 mAh cm^(-2)up to date.The 3D-printed porous frameworks featuring the multidirectional transport of Li ion and superior affinity of electrolyte,exceptionally boost active material utilization and fast electrochemical kinetics of thick electrodes,resulting in a high specific capacity of 208 mAh g^(-1).Furthermore,the printed electrode has a capacity retention rate of 88%after 150 cycles at 2 C.A full cell assembled with a printed NCM811 cathode and graphite anode shows high energy density of 417 Wh kg^(-1)at electrode level and long-term cyclability.This work provides an effective strategy for fabricating long-lifespan and high-energy-density lithium-ion batteries.
基金supported by the Fundamental Research Funds for the Central Universities(XK1802-2)the National Key Basic Research Program of China(973 Program,2014CB643604)+2 种基金the National Natural Science Foundation of China(51673017)National Natural Science Foundation of China(21404005)the Natural Science Foundation of Jiangsu Province(BK20150273)。
文摘LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)material,as the promising cathode candidate for next-generation highenergy lithium-ion batteries,has gained considerable attention for extremely high theoretical capacity and low cost.Nevertheless,the intrinsic drawbacks of NCM811 such as unstable structure and inevitable interface side reaction result in severe capacity decay and thermal runaway.Herein,a novel polyimide(denoted as PI-Om DT)constructed with the highly polar and micro-branched crosslinking network is reported as a binder material for NCM811 cathode.The micro-branched crosslinking network is achieved by using 1,3,5-Tris(4-aminophenoxy)benzene(TAPOB)as a crosslinker via condensation reaction,which endows excellent mechanical properties and large free volume.Meanwhile,the massive polar carboxyl(-COOH)groups provide strong adhesion sites to active NCM811 particles.These functions of PIOm DT binder collaboratively benefit to forming the mechanically robust and homogeneous coating layer with rapid Li+diffusion on the surface of NCM811,significantly stabilizing the cathode structure,suppressing the detrimental interface side reaction and guaranteeing the shorter ion-diffusion and electron-transfer paths,consequently enhancing electrochemical performance.As compared to the NCM811 with PVDF binder,the NCM811 using PI-Om DT binder delivers a superior high-rate capacity(121.07 vs.145.38 m Ah g^(-1))at 5 C rate and maintains a higher capacity retention(80.38%vs.91.6%)after100 cycles at 2.5–4.3 V.Particularly,at the high-voltage conditions up to 4.5 and 4.7 V,the NCM811 with PI-Om DT binder still maintains the remarkable capacity retention of 88.86%and 72.5%after 100 cycles,respectively,paving the way for addressing the high-voltage operating stability of the NCM811 cathode.Moreover,the full-charged NCM811 cathode with PI-Om DT binder exhibits a significantly enhanced thermal stability,improving the safety performance of batteries.This work opens a new avenue for developing high-energy NCM811 based lithium-ion batteries with long cycle-life and superior safety performance using a novel and effective binder.
基金supported by the National Natural Science Foundation of China(52072036)the Key Research and Development Program of Henan province,China(231111242500).
文摘With the widespread use of lithium-ion batteries in electric vehicles,energy storage,and mobile terminals,there is an urgent need to develop cathode materials with specific properties.However,existing material control synthesis routes based on repetitive experiments are often costly and inefficient,which is unsuitable for the broader application of novel materials.The development of machine learning and its combination with materials design offers a potential pathway for optimizing materials.Here,we present a design synthesis paradigm for developing high energy Ni-rich cathodes with thermal/kinetic simulation and propose a coupled image-morphology machine learning model.The paradigm can accurately predict the reaction conditions required for synthesizing cathode precursors with specific morphologies,helping to shorten the experimental duration and costs.After the model-guided design synthesis,cathode materials with different morphological characteristics can be obtained,and the best shows a high discharge capacity of 206 mAh g^(−1)at 0.1C and 83%capacity retention after 200 cycles.This work provides guidance for designing cathode materials for lithium-ion batteries,which may point the way to a fast and cost-effective direction for controlling the morphology of all types of particles.
基金financially supported by the National Natural Science Foundation of China(Nos.52072208,52402124,and 52302278)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110531)+1 种基金Supported by the Postdoctoral Fellowship Program(GradeB)of China Postdoctoral Science Foundation under Grant Number GZB20250057China Postdoctoral Science Foundation(2025M770223).
文摘LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),a high-nickel layered oxide,has emerged as a frontrunner for next-generation lithium-ion batteries(LIBs)due to its high energy density,excellent rate performance,and cost-effectiveness.However,NCM811 cathodes face multifaceted challenges,including cation mixing,microcracking,and residual lithium compounds,necessitating a comprehensive understanding for addressing these critical issues.In this review,we provide an in-depth analysis of recent advancements,presenting actionable insights into effective strategies to address the key issues in the NCM811 cathode and proposing pathways for optimizing NCM811 cathodes in LIB applications.Additionally,the forward-looking perspectives are explored in this review,highlighting the role of advanced material characterization techniques,theoretical modeling,and computational simulations in overcoming the inherent limitations of NCM811 cathodes.By synthesizing current knowledge and technological advancements,this review aims to serve as a foundational resource for researchers and industry professionals striving to enhance the performance and accelerate the commercialization of NCM811 cathode materials,contributing to the future of energy storage solutions.
文摘At present,lithium-ion batteries(LIBs)have been vastly applied and are widely being used for portable device,hybrid electric vehicles,and aviation field.Cathode materials,as the most important part in the LIBs,shows a profound prospect and potential.This study mainly focuses on the study of the means of how to improve the electrochemical properties and performance of the NCM cathode materials,examining the characterization of the NCM cathode materials through the characterization techniques.By referring different doping elements on NCM cathode materials,this paper aims to examine the structural properties,electrochemical performance,and stability of these materials under different dopants.Several characterization techniques,inductively coupled plasma(ICP),x-ray photoelectron spectroscope(XPS),Scanning electron microscopy(SEM),transmission electron microscopy(TEM),energy dispersive spectroscope(EDS),and x-ray diffraction(XRD)results have clearly displayed a large amount of figure on cathode materials,which help us to gain a better understanding on the characteristic of each cathode materials and help us to do the further calculation and study on cathode materials.
基金This study was supported by BASF SE.F Strauss acknowledges financial support from the Fonds der Chemischen Industrie through a Liebig fellowship.
文摘Solid-state batteries(SSBs)are a promising next step in electrochemical energy storage but are plagued by a number of problems.In this study,we demonstrate the recurring issue of mechanical degradation because of volume changes in layered Ni-rich oxide cathode materials in thiophosphate-based SSBs.Specifically,we explore superionic solid electrolytes(SEs)of different crystallinity,namely glassy 1.5Li_(2)S-0.5P_(2)S_(5)-LiI and argyrodite Li_(6)PS_(5)Cl,with emphasis on how they affect the cyclability of slurry-cast cathodes with NCM622(60%Ni)or NCM851005(85%Ni).The application of a combination of ex situ and in situ analytical techniques helped to reveal the benefits of using a SE with a low Young’s modulus.Through a synergistic interplay of(electro)chemical and(chemo)mechanical effects,the glassy SE employed in this work was able to achieve robust and stable interfaces,enabling intimate contact with the cathode material while at the same time mitigating volume changes.Our results emphasize the importance of considering chemical,electrochemical,and mechanical properties to realize long-term cycling performance in high-loading SSBs.
基金National Natural Science Foundation of China,Grant/Award Numbers:51974256,52034011The Outstanding Young Scholars of Shaanxi,Grant/Award Number:2019JC-12+3 种基金The Natural Science Basic Research Plan in Shaanxi Province of China,Grant/Award Numbers:2019JLZ-01,2019JLM-29Fundamental Research Funds for the Central Universities,Grant/Award Numbers:3102021ZD0401,3102021TS0406,3102019JC005the Youth Innovation Team of Shaanxi UniversitiesND Basic Research Funds,Grant/Award Number:G2022WD。
文摘Promoting industry applications of high-energy Li metal batteries(LMBs)is of vital importance for accelerating the electrification and decarbonization of our society.Unfortunately,the time-dependent storage aging of Ah-level Li metal pouch cells,a ubiquitous but crucial practical indicator,has not yet been revealed.Herein,we first report the storage behaviors and multilateral synergistic aging mechanism of Ah-level NCM811jjLi pouch cells during the 120-day long-term storage under various conditions.Contrary to the conventional belief of Li-ion batteries with graphite intercalation anodes,the significant available capacity loss of 32.8%on average originates from the major electrolyte-sensitive anode corrosion and partial superimposed cathode degradation,and the irreversible capacity loss of 13.3%is essentially attributed to the unrecoverable interface/structure deterioration of NCM with further hindrance of the aged Li.Moreover,principles of alleviating aging have been proposed.This work bridges academia and industry and enriches the fundamental epistemology of storage aging of LMBs,shedding light on realistic applications of high-energy batteries.
