Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and l...Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.展开更多
Efficient and reliable energy storage systems are crucial for our modern society.Lithium-ion batteries(LIBs)with excellent performance are widely used in portable electronics and electric vehicles(EVs),but frequent fi...Efficient and reliable energy storage systems are crucial for our modern society.Lithium-ion batteries(LIBs)with excellent performance are widely used in portable electronics and electric vehicles(EVs),but frequent fires and explosions limit their further and more widespread applications.This review summarizes aspects of LIB safety and discusses the related issues,strategies,and testing standards.Specifically,it begins with a brief introduction to LIB working principles and cell structures,and then provides an overview of the notorious thermal runaway,with an emphasis on the effects of mechanical,electrical,and thermal abuse.The following sections examine strategies for improving cell safety,including approaches through cell chemistry,cooling,and balancing,afterwards describing current safety standards and corresponding tests.The review concludes with insights into potential future developments and the prospects for safer LIBs.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
Severe capacity fading and poor high rate performance of lithium sulfur(Li–S) battery caused by "shuttle effect" and low conductivity of sulfur hampers its further developments and applications. Li_4Ti_5O_(...Severe capacity fading and poor high rate performance of lithium sulfur(Li–S) battery caused by "shuttle effect" and low conductivity of sulfur hampers its further developments and applications. Li_4Ti_5O_(12) (LTO)possesses high lithium ion conductivity, and it is also can be used as an active adsorbent for polysulfide. Herein, fine LTO particle coated carbon nanofibers(CNF) were prepared and a conductive network both for electron and lithium ion was built, which can greatly promote the electrochemical conversion of polysulfide and improve the rate performance of Li–S batteries. Meanwhile, a quantity of adsorption sites is constructed by defects of the surface of LTO-CNF membrane to effectively immobilize polysulfide. The multifunctional LTO-CNF interlayer could impede the shuttle effect and enhance comprehensive electrochemical performance of Li–S batteries, especially high rate performance. With such LTO-CNF interlayer,the Li–S battery presents a specific capacity of 641.9 mAh/g at 5 C rate. After 400 cycles at 1 C, a capacity of 618.0 mAh/g is retained. This work provides a feasible strategy to achieve high performance of Li–S battery for practical utilization.展开更多
Through tailoring interfacial chemistry,electrolyte engineering is a facile yet effective strategy for highperformance lithium(Li)metal batteries,where the solvation structure is critical for interfacial chemistry.Her...Through tailoring interfacial chemistry,electrolyte engineering is a facile yet effective strategy for highperformance lithium(Li)metal batteries,where the solvation structure is critical for interfacial chemistry.Herein,the effect of electrostatic interaction on regulating an anion-rich solvation is firstly proposed.The moderate electrostatic interaction between anion and solvent promotes anion to enter the solvation sheath,inducing stable solid electrolyte interphase with fast Li+transport kinetics on the anode.This asdesigned electrolyte exhibits excellent compatibility with Li metal anode(a Li deposition/stripping Coulombic efficiency of 99.3%)and high-voltage LiCoO_(2) cathode.Consequently,the 50μm-thin Li||high-loading LiCoO_(2) cells achieve significantly improved cycling performance under stringent conditions of high voltage over 4.5 V,lean electrolyte,and wide temperature range(-20 to 60℃).This work inspires a groundbreaking strategy to manipulate the solvation structure through regulating the interactions of solvent and anion for highperformance Li metal batteries.展开更多
Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs...Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.展开更多
The rapid advancement in electronic devices,electric vehicles,and grid storage stations have lead to a high demand for energy storage devices with enhanced power and energy densities as well as extended lifespans.Lith...The rapid advancement in electronic devices,electric vehicles,and grid storage stations have lead to a high demand for energy storage devices with enhanced power and energy densities as well as extended lifespans.Lithium ion hybrid capacitors are constructed with battery-type anodes and capacitor-type cathodes,which enables the direct integration of the high energy from lithium ion batteries and high power and long lifetime from supercapacitors,making lithium ion hybrid capacitor one of the most promising energy storage devices.In the past two decades,tremendous efforts have been put into the search for suitable battery-type anode materials with improved Faradaic reaction kinetics so that it can match with the fast non-Faradaic charging rate of the capacitive cathodes.This review aims to provide an up-to-date and comprehensive summary of the battery-type anode materials for high-performance lithium ion hybrid capacitors.To date,a large variety of battery-type anode materials have been explored with smart material design strategies,such as carbonaceous materials,metal oxides,alloys,sulfides,nitirdes,and Mxenes,etc.,which will be discussed in detail.A perspective to the challenges and future developing trends of lithium ion hybrid capacitors is proposed to close.展开更多
It remains challenging to effectively estimate the remaining capacity of the secondary lithium-ion batteries that have been widely adopted for consumer electronics,energy storage,and electric vehicles.Herein,by integr...It remains challenging to effectively estimate the remaining capacity of the secondary lithium-ion batteries that have been widely adopted for consumer electronics,energy storage,and electric vehicles.Herein,by integrating regular real-time current short pulse tests with data-driven Gaussian process regression algorithm,an efficient battery estimation has been successfully developed and validated for batteries with capacity ranging from 100%of the state of health(SOH)to below 50%,reaching an average accuracy as high as 95%.Interestingly,the proposed pulse test strategy for battery capacity measurement could reduce test time by more than 80%compared with regular long charge/discharge tests.The short-term features of the current pulse test were selected for an optimal training process.Data at different voltage stages and state of charge(SOC)are collected and explored to find the most suitable estimation model.In particular,we explore the validity of five different machine-learning methods for estimating capacity driven by pulse features,whereas Gaussian process regression with Matern kernel performs the best,providing guidance for future exploration.The new strategy of combining short pulse tests with machine-learning algorithms could further open window for efficiently forecasting lithium-ion battery remaining capacity.展开更多
Implementation of sodium metal anode is highly desired for sodium batteries due to its high theoretical capacity and low redox potential.Unfortunately,formation of unstable solid electrolyte interphase(SEI)and uncontr...Implementation of sodium metal anode is highly desired for sodium batteries due to its high theoretical capacity and low redox potential.Unfortunately,formation of unstable solid electrolyte interphase(SEI)and uncontrollable growth of dendrites during charge/discharge cycles greatly hinder the practical application of sodium metal anode.In this study,an organic-metal artificial layer made of PVdF and Bi was constructed to protect Cu current collector via a facile coating method,leading to smooth and dense sodium plating/stripping,which in retern enables stable cycling and high coulombic efficiency(CE).At 1 mA cm^(−2),PB@Cu current collector presents extended lifetime of~2500 h with high sodium utilization of 50%,which is approximately six times higher than Cu current collector.PB@Cu electrode also displays high average CE of 99.92%and 99.95%over 2500 and 1300 cycles at 1 and 2 mA cm^(−2) respectively,which is in sharp contrast to the low and tremendously fluctuant CE gained from bare Cu electrode.Moreover,stable capacity of>90 mAh g^(−1) over 150 cycles is realized for PB@Cu-based full cell assembled with NVP cathode at a low negative-positive capacity ratio of~3.5,which is significantly higher than 37.2 mAh g^(−1) obtained from NVP/Cu at 150th cycle.The superior electrochemical performance of PB@Cu current collector is revealed to originate from the alloyed Na_(3)Bi phase with high sodium conductivity and robust mechanical strength as well as the formation of NaF-rich SEI with fast sodium ion migration,which enable dendrite-free morphology during plating/stripping cycles.展开更多
The development of advanced lithium batteries represents a major technological challenge for the new century.Understanding the fundamental electrode degradation mechanisms is important for battery performance improvem...The development of advanced lithium batteries represents a major technological challenge for the new century.Understanding the fundamental electrode degradation mechanisms is important for battery performance improvements.The complex electrochemical processes inside a working battery are being explored to a limited extent.Various advanced material characterization techniques have been used to monitor dynamic conditions for optimizing battery materials.State-of-the-art atomic force microscopy methods have been applied to energy storage systems,specifically lithium-ion batteries.Atomic force microscopy is an ideal tool to provide localized morphological,chemical,and physical information at nanoscale for the in-depth understanding of the electrochemical processes,reaction mechanisms,and degradation of battery materials.Here,we review recent progress in the development and application of atomic force microscopy for high-performance lithium-ion batteries.We discuss atomic force microscopy as an analytical tool to help researchers understand graphite,silicon,layered metal oxides,and other representative electrode materials.We summarize the importance of atomic force microscopy technique in studying the next-generation Li–S and Li–O 2 batteries.We also highlight some of the remaining challenges and possible solutions for future development.展开更多
Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the ...Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the aforementioned problems using a facile method under mild conditions.Polycarbonate diol(PCDL),triethanolamine(TEA) and hexamethylene diisocyanate(HDI) were chosen as precursors to prepare the cross-linked binder.The in-situ polymerized binder(PTH) builds a strong network in sulfur cathode,which could restrain the volume expansion of sulfu r.Moreover,by adopting functional groups of oxygen atoms and nitrogen atoms,the binder could effectively facilitate transportation of Li-ion and adsorb polysulfide chemically.The Li-S battery with bare sulfur and carbon/sulfur composite cathodes and cross-linked PTH binder displays much better electrochemical performance than that of the battery with PVDF.The PTH-bare S cathode with a mass loading of 5.97 mg/cm^2 could deliver a capacity of 733.3 mAh/g at 0.2 C,and remained 585.5 mAh/g after 100 cycles.This in-situ polymerized binder is proved to be quite effective on restraining the volume expansion and suppressing polysulfide shuttle effect,then improving the electrochemical performance of Li-S battery.展开更多
It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs wher...It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs where the barrier to recycling is economical,and to make recycling more feasible,it is required that the value of the processed recycled material exceeds the value of raw commodity materials.The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials.This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums,thereby significantly improving the economic profitability of LIB recycling.Organolithiums(R-O-Li and R-Li)were prepared using alkyl alcohol(R-OH)and alkyl bromide(R-Br)as substrates,where R includes varying hindered alkyl hydrocarbons.The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between$29.5 and$226.5 kg^(−1) cell.The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials,improving the profitability of recycling LIBs over traditional pyrometallurgical($0.86 kg^(−1) cell),hydrometallurgical($1.00 kg^(−1) cell),and physical direct recycling methods($5.40 kg^(−1) cell).展开更多
Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfort...Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfortunately,the intractable dendritic Li deposition during cycling greatly restrains the large-scale applications of Li metal anodes.Recent advances have been explored to address this issue,among which a specific class of electrolyte additives for electroplating is deeply impressive,as they are economic and pragmatic.Different from the conventional additives that construct solid electrolyte interphase(SEI)layer on anodes,they make dendrite-free Li metal anodes feasible through altering Li plating behavior.In this research news article,the interlinked principles between industrial electroplating and Li deposition are firstly illustrated.The featured effects of electroplating additives on regulating Li plating morphology are also summarized and mainly divided into three categories:co-deposition with Li cation,coordination with Li cation,and leveling effect of Li films.Furthermore,the mechanism exploration or derivative use of electroplating additive for dendrite suppression and potential research directions are proposed,with emphasizing that industrial electroplating might enable Li metal anode to scalable battery techniques and spread to metal battery systems beyond Li.展开更多
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.展开更多
The energy density of commercial lithium(Li)ion batteries with graphite anode is reaching the limit.It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density t...The energy density of commercial lithium(Li)ion batteries with graphite anode is reaching the limit.It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent.However,the poor reversibility and infinite volume change of Li metal hinder the realistic implementation of Li metal in battery community.Herein,a commercially viable hybrid Li-ion/metal battery is realized by a coordinated strategy of symbiotic anode and prelithiated cathode.To be specific,a scalable template-removal method is developed to fabricate the porous graphite layer(PGL),which acts as a symbiotic host for Li ion intercalation and subsequent Li metal deposition due to the enhanced lithiophilicity and sufficient ion-conducting pathways.A continuous dissolution-deintercalation mechanism during delithiation process further ensures the elimination of dead Li.As a result,when the excess plating Li reaches 30%,the PGL could deliver an ultrahigh average Coulombic efficiency of 99.5% for 180 cycles with a capacity of 2.48 m Ah cm^(-2) in traditional carbonate electrolyte.Meanwhile,an air-stable recrystallized lithium oxalate with high specific capacity(514.3 m Ah g^(-1))and moderate operating potential(4.7-5.0 V)is introduced as a sacrificial cathode to compensate the initial loss and provide Li source for subsequent cycles.Based on the prelithiated cathode and initial Li-free symbiotic anode,under a practical-level3 m Ah capacity,the assembled hybrid Li-ion/metal full cell with a P/N ratio(capacity ratio of Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2) to graphite)of 1.3exhibits significantly improved capacity retention after 300 cycles,indicating its great potential for high-energy-density Li batteries.展开更多
In this work, the electrochemical performance of LiNi0.8Co0.1Mn0.1O2(NCM811) has been investigated after cycling with various upper cutoff voltages. Noteworthily, electrochemical impedance of NCM811 declined with the ...In this work, the electrochemical performance of LiNi0.8Co0.1Mn0.1O2(NCM811) has been investigated after cycling with various upper cutoff voltages. Noteworthily, electrochemical impedance of NCM811 declined with the increasing cycle number to high voltages. It was found that the decline of charge transfer impedance could be related to the structural and compositional change of cathode electrolyte interphase(CEI) of NCM811 when charging to high voltages, based on the characterization of electrochemical impedance spectroscopy(EIS), X-ray photoelectron spectroscopy(XPS) and transmission electron microscopy(TEM). The corresponding mechanism has also been proposed in this study. Specifically, due to the increasing roughness of cathode surface, the bottom of CEI film and cubic phase on cathode surface form a transition region mainly at high voltages, leading to the nonobvious boundary. This newly formed transition region at high voltages could promote the Li ion diffusion from electrolyte to cathode, then reducing charge transfer impedance. Additionally, the decrease of Li F on the surface of the cathode could also make a contribution to lower the interface impedance. This study delivers a different evolution of CEI on NCM811, and the impact of CEI evolution on electrochemical performance when charging to a high voltage.展开更多
Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-dens...Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.展开更多
Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder the...Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder their practical applications.Functional gradient material(FGM)design endows the electrode materials with property gradient,thus providing great opportunities to address the kinetics and stability obstacles.To date,still no review or perspective has covered recent advancements in gradient design at multiple scales for boosting lithium battery performances.To fill this void,this work provides a timely and comprehensive overview of this exciting and sustainable research field.We begin by overviewing the fundamental features of FGM and the rationales of gradient design for improved electrochemical performance.Then,we comprehensively review FGM design for rechargeable lithium batteries at various scales,including natural or artificial solid electrolyte interphase(SEI)at the nanoscale,micrometer-scale electrode particles,and macroscale electrode films.The link between gradient structure design and improved electrochemical performance is particularly highlighted.The most recent research into constructing novel functional gradients,such as valence and temperature gradients,has also been explored.Finally,we discussed the current constraints and future scope of FGM in rechargeable lithium batteries,aiming to inspire the development of novel FGM for next-generation high-performance lithium batteries.展开更多
Advanced electrolyte engineering is an important strategy for developing high-efficacy lithium(Li)metal batteries(LMBs).Unfortunately,the current electrolytes limit the scope for creating batteries that perform well o...Advanced electrolyte engineering is an important strategy for developing high-efficacy lithium(Li)metal batteries(LMBs).Unfortunately,the current electrolytes limit the scope for creating batteries that perform well over temperature ranges.Here,we present a new electrolyte design that uses fluorosulfonyl carboxylate as a non-solvating solvent to form difluoroxalate borate(DFOB-)anion-rich solvation sheath,to realize high-performance working of temperature-tolerant LMBs.With this optimized electrolyte,favorable SEI and CEI chemistries on Li metal anode and nickel-rich cathode are achieved,respectively,leading to fast Li^(+)transfer kinetics,dendrite-free Li deposition and suppressed electrolyte deterioration.Therefore,Li||LiNi_(0.80)Co_(0.15)Al_(0.05)O_(2)batteries with a thin Li foil(50μm)show a long-term cycling lifespan over 400 cycles at 1C and a superior capacity retention of 90%after 200 cycles at 0.5C under 25℃.Moreover,this electrolyte extends the operating temperature from-10 to 30℃and significantly improve the capacity retention and Coulombic efficiency of batteries are improved at high temperature(60℃).Fluorosulfonyl carboxylates thus have considerable potential for use in high-performance and allweather LMBs,which broadens the new exploring of electrolyte design.展开更多
Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that...Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that is stable in ambient air with an average operating voltage of~3.8 V,demonstrating excellent cycling stability with a capacity retention of more than 92.7%after 500 cycles at 20 mA g^(-1) and good rate capability with 91.9%capacity utilization at 500 mA g^(-1) with respect to capacity at 5 mA g^(-1) between 2.0 and 4.0 V.When the upper cutoff voltage is increased to 4.4 V,P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) delivers a reversible capacity of 71.9 mAh g^(-1) and retains 91.8%of the capacity after 100 cycles at 20 mA g^(-1).The charge compensation during charge/discharge is mainly due to the redox couple of Ni^(2+)/Ni^(3+)in the host with a small amount of contribution from oxygen.The stable structure of the material without phase transformation and with small volume change during charge-discharge allows it to give excellent cycle performance especially when the upper cutoff voltage is not higher than 4.2 V.展开更多
基金supported by the Yunnan Fundamental Research Projects(Grant Nos.202401AU070163 and 202501AT070298)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)+5 种基金the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Expert Workstation Support Project of Yunnan Province(Grant No.202405AF140069)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Test Foundation of Kunming University of Science and Technology(Grant No.2023T20220122)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2025QN02057)the Ordos City Strategic Pioneering Science and Technology Special Program for New Energy(Grant No.DC2400003365).
文摘Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.
基金financially supported by the National Key Basic Research Program of China(No.2014CB932400)the Joint Fund of the National Natural Science Foundation of China(No.U1401243)+3 种基金the National Natural Science Foundation of China(No.51232005)the Shenzhen Technical Plan Project(No.JCYJ20150529164918735,CYJ20170412170911187,KQJSCX20160226191136)the Guangdong Technical Plan Project(No.2015TX01N011)the financial support by Bio4Energy program。
文摘Efficient and reliable energy storage systems are crucial for our modern society.Lithium-ion batteries(LIBs)with excellent performance are widely used in portable electronics and electric vehicles(EVs),but frequent fires and explosions limit their further and more widespread applications.This review summarizes aspects of LIB safety and discusses the related issues,strategies,and testing standards.Specifically,it begins with a brief introduction to LIB working principles and cell structures,and then provides an overview of the notorious thermal runaway,with an emphasis on the effects of mechanical,electrical,and thermal abuse.The following sections examine strategies for improving cell safety,including approaches through cell chemistry,cooling,and balancing,afterwards describing current safety standards and corresponding tests.The review concludes with insights into potential future developments and the prospects for safer LIBs.
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supported by the National Key Basic Research Program of China (2014CB932400)the National Natural Science Foundation of China (51672156 and 51232005)+3 种基金Guangdong special support program (2015TQ01N401)Guangdong Province Technical Plan Project (2017B010119001 and 2017B090907005)Dongguan City (2015509119213)Shenzhen Technical Plan Project (JCYJ20170817161221958, JCYJ20170412170706047, JCYJ20170307153806471, and GJHS20170314165324888)
文摘Severe capacity fading and poor high rate performance of lithium sulfur(Li–S) battery caused by "shuttle effect" and low conductivity of sulfur hampers its further developments and applications. Li_4Ti_5O_(12) (LTO)possesses high lithium ion conductivity, and it is also can be used as an active adsorbent for polysulfide. Herein, fine LTO particle coated carbon nanofibers(CNF) were prepared and a conductive network both for electron and lithium ion was built, which can greatly promote the electrochemical conversion of polysulfide and improve the rate performance of Li–S batteries. Meanwhile, a quantity of adsorption sites is constructed by defects of the surface of LTO-CNF membrane to effectively immobilize polysulfide. The multifunctional LTO-CNF interlayer could impede the shuttle effect and enhance comprehensive electrochemical performance of Li–S batteries, especially high rate performance. With such LTO-CNF interlayer,the Li–S battery presents a specific capacity of 641.9 mAh/g at 5 C rate. After 400 cycles at 1 C, a capacity of 618.0 mAh/g is retained. This work provides a feasible strategy to achieve high performance of Li–S battery for practical utilization.
基金supported by National Nature Science Foundation of China(No.51872157 and No.52072208)National Key R&D Program of China 2021YFA1202802Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N111)。
文摘Through tailoring interfacial chemistry,electrolyte engineering is a facile yet effective strategy for highperformance lithium(Li)metal batteries,where the solvation structure is critical for interfacial chemistry.Herein,the effect of electrostatic interaction on regulating an anion-rich solvation is firstly proposed.The moderate electrostatic interaction between anion and solvent promotes anion to enter the solvation sheath,inducing stable solid electrolyte interphase with fast Li+transport kinetics on the anode.This asdesigned electrolyte exhibits excellent compatibility with Li metal anode(a Li deposition/stripping Coulombic efficiency of 99.3%)and high-voltage LiCoO_(2) cathode.Consequently,the 50μm-thin Li||high-loading LiCoO_(2) cells achieve significantly improved cycling performance under stringent conditions of high voltage over 4.5 V,lean electrolyte,and wide temperature range(-20 to 60℃).This work inspires a groundbreaking strategy to manipulate the solvation structure through regulating the interactions of solvent and anion for highperformance Li metal batteries.
基金supported by the National Natural Science Foundation of China(Nos.51872157,52072208)Shenzhen Technical Plan Project(JCYJ20170817161753629)+1 种基金Fundamental Research Project of Shenzhen(No.JCYJ20190808153609561)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N111).
文摘Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.
基金This work was supported by National Key Basic Research Program of China(No.2014CB932400)Joint Fund of the National Natural Science Foundation of China(No.U1401243)+2 种基金National Nature Science Foundation of China(No.51232005,51571144)Shenzhen Tech-nical Plan Project(No.JCYJ20150529164918735,JCYJ20170412170911187,KQJSCX20160226191136)Guangdong Technical Plan Project(No.2015T X01N011).
文摘The rapid advancement in electronic devices,electric vehicles,and grid storage stations have lead to a high demand for energy storage devices with enhanced power and energy densities as well as extended lifespans.Lithium ion hybrid capacitors are constructed with battery-type anodes and capacitor-type cathodes,which enables the direct integration of the high energy from lithium ion batteries and high power and long lifetime from supercapacitors,making lithium ion hybrid capacitor one of the most promising energy storage devices.In the past two decades,tremendous efforts have been put into the search for suitable battery-type anode materials with improved Faradaic reaction kinetics so that it can match with the fast non-Faradaic charging rate of the capacitive cathodes.This review aims to provide an up-to-date and comprehensive summary of the battery-type anode materials for high-performance lithium ion hybrid capacitors.To date,a large variety of battery-type anode materials have been explored with smart material design strategies,such as carbonaceous materials,metal oxides,alloys,sulfides,nitirdes,and Mxenes,etc.,which will be discussed in detail.A perspective to the challenges and future developing trends of lithium ion hybrid capacitors is proposed to close.
基金support from Shenzhen Municipal Development and Reform Commission(Grant Number:SDRC[2016]172)Shenzhen Science and Technology Program(Grant No.KQTD20170810150821146)Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School,and Shanghai Shun Feng Machinery Co.,Ltd.
文摘It remains challenging to effectively estimate the remaining capacity of the secondary lithium-ion batteries that have been widely adopted for consumer electronics,energy storage,and electric vehicles.Herein,by integrating regular real-time current short pulse tests with data-driven Gaussian process regression algorithm,an efficient battery estimation has been successfully developed and validated for batteries with capacity ranging from 100%of the state of health(SOH)to below 50%,reaching an average accuracy as high as 95%.Interestingly,the proposed pulse test strategy for battery capacity measurement could reduce test time by more than 80%compared with regular long charge/discharge tests.The short-term features of the current pulse test were selected for an optimal training process.Data at different voltage stages and state of charge(SOC)are collected and explored to find the most suitable estimation model.In particular,we explore the validity of five different machine-learning methods for estimating capacity driven by pulse features,whereas Gaussian process regression with Matern kernel performs the best,providing guidance for future exploration.The new strategy of combining short pulse tests with machine-learning algorithms could further open window for efficiently forecasting lithium-ion battery remaining capacity.
基金the support from the Shenzhen Natural Science Fund(the Stable Support Plan Program GXWD20201230155427003-20200824094017001)。
文摘Implementation of sodium metal anode is highly desired for sodium batteries due to its high theoretical capacity and low redox potential.Unfortunately,formation of unstable solid electrolyte interphase(SEI)and uncontrollable growth of dendrites during charge/discharge cycles greatly hinder the practical application of sodium metal anode.In this study,an organic-metal artificial layer made of PVdF and Bi was constructed to protect Cu current collector via a facile coating method,leading to smooth and dense sodium plating/stripping,which in retern enables stable cycling and high coulombic efficiency(CE).At 1 mA cm^(−2),PB@Cu current collector presents extended lifetime of~2500 h with high sodium utilization of 50%,which is approximately six times higher than Cu current collector.PB@Cu electrode also displays high average CE of 99.92%and 99.95%over 2500 and 1300 cycles at 1 and 2 mA cm^(−2) respectively,which is in sharp contrast to the low and tremendously fluctuant CE gained from bare Cu electrode.Moreover,stable capacity of>90 mAh g^(−1) over 150 cycles is realized for PB@Cu-based full cell assembled with NVP cathode at a low negative-positive capacity ratio of~3.5,which is significantly higher than 37.2 mAh g^(−1) obtained from NVP/Cu at 150th cycle.The superior electrochemical performance of PB@Cu current collector is revealed to originate from the alloyed Na_(3)Bi phase with high sodium conductivity and robust mechanical strength as well as the formation of NaF-rich SEI with fast sodium ion migration,which enable dendrite-free morphology during plating/stripping cycles.
文摘The development of advanced lithium batteries represents a major technological challenge for the new century.Understanding the fundamental electrode degradation mechanisms is important for battery performance improvements.The complex electrochemical processes inside a working battery are being explored to a limited extent.Various advanced material characterization techniques have been used to monitor dynamic conditions for optimizing battery materials.State-of-the-art atomic force microscopy methods have been applied to energy storage systems,specifically lithium-ion batteries.Atomic force microscopy is an ideal tool to provide localized morphological,chemical,and physical information at nanoscale for the in-depth understanding of the electrochemical processes,reaction mechanisms,and degradation of battery materials.Here,we review recent progress in the development and application of atomic force microscopy for high-performance lithium-ion batteries.We discuss atomic force microscopy as an analytical tool to help researchers understand graphite,silicon,layered metal oxides,and other representative electrode materials.We summarize the importance of atomic force microscopy technique in studying the next-generation Li–S and Li–O 2 batteries.We also highlight some of the remaining challenges and possible solutions for future development.
基金supported by the National Natural Science Foundation of China(No.51672156)Guangdong special support program(No.2015TQ01 N401)+2 种基金Guangdong Province Technical Plan Project(Nos.2017B010119001 and 20178090907005)Shenzhen Technical Plan Project(Nos.JCYJ20170412170706047,JCYJ20170307153806471 and GJHS20170314165324888)Shenzhen Graphene Manufacturing Innovation Center(No.201901161513)。
文摘Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the aforementioned problems using a facile method under mild conditions.Polycarbonate diol(PCDL),triethanolamine(TEA) and hexamethylene diisocyanate(HDI) were chosen as precursors to prepare the cross-linked binder.The in-situ polymerized binder(PTH) builds a strong network in sulfur cathode,which could restrain the volume expansion of sulfu r.Moreover,by adopting functional groups of oxygen atoms and nitrogen atoms,the binder could effectively facilitate transportation of Li-ion and adsorb polysulfide chemically.The Li-S battery with bare sulfur and carbon/sulfur composite cathodes and cross-linked PTH binder displays much better electrochemical performance than that of the battery with PVDF.The PTH-bare S cathode with a mass loading of 5.97 mg/cm^2 could deliver a capacity of 733.3 mAh/g at 0.2 C,and remained 585.5 mAh/g after 100 cycles.This in-situ polymerized binder is proved to be quite effective on restraining the volume expansion and suppressing polysulfide shuttle effect,then improving the electrochemical performance of Li-S battery.
基金National Natural Science Foundation of China,Grant/Award Number:51232005Key-Area Research and Development Program of Guangdong Province,Grant/Award Number:2020B090919003+1 种基金Joint Fund of the National Natural Science Foundation of China,Grant/Award Number:U1401243Shenzhen Technical Plan Project,Grant/Award Number:CYJ20170412170911187。
文摘It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs where the barrier to recycling is economical,and to make recycling more feasible,it is required that the value of the processed recycled material exceeds the value of raw commodity materials.The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials.This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums,thereby significantly improving the economic profitability of LIB recycling.Organolithiums(R-O-Li and R-Li)were prepared using alkyl alcohol(R-OH)and alkyl bromide(R-Br)as substrates,where R includes varying hindered alkyl hydrocarbons.The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between$29.5 and$226.5 kg^(−1) cell.The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials,improving the profitability of recycling LIBs over traditional pyrometallurgical($0.86 kg^(−1) cell),hydrometallurgical($1.00 kg^(−1) cell),and physical direct recycling methods($5.40 kg^(−1) cell).
基金support from National Nature Science Foundation of China(Grant No.51872157)Shenzhen Technical Plan Project(Grant Nos.JCYJ20170412170911187 and JCYJ20170817161753629)+1 种基金Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(Grant No.2017BT01N111)Guangdong Technical Plan Project(Grant No.2017B090907005)
文摘Lithium(Li)metal batteries have long been deemed as the representative high-energy-density energy storage systems due to the ultrahigh theoretical capacity and lowest electrochemical potential of Li metal anode.Unfortunately,the intractable dendritic Li deposition during cycling greatly restrains the large-scale applications of Li metal anodes.Recent advances have been explored to address this issue,among which a specific class of electrolyte additives for electroplating is deeply impressive,as they are economic and pragmatic.Different from the conventional additives that construct solid electrolyte interphase(SEI)layer on anodes,they make dendrite-free Li metal anodes feasible through altering Li plating behavior.In this research news article,the interlinked principles between industrial electroplating and Li deposition are firstly illustrated.The featured effects of electroplating additives on regulating Li plating morphology are also summarized and mainly divided into three categories:co-deposition with Li cation,coordination with Li cation,and leveling effect of Li films.Furthermore,the mechanism exploration or derivative use of electroplating additive for dendrite suppression and potential research directions are proposed,with emphasizing that industrial electroplating might enable Li metal anode to scalable battery techniques and spread to metal battery systems beyond Li.
基金supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
基金the support by the Key-Area Research and Development Program of Guangdong Province(No.2020B090919003)the National Nature Science Foundation of China(Nos.51872157 and 52072208)+4 种基金the Shenzhen Technical Plan Project(Nos.JCYJ20170817161753629 and JCYJ20170412170911187)the Special Fund Project for Strategic Emerging Industry Development of Shenzhen(No.20170428145209110)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01N111)the Support Plan for Shenzhen Manufacturing Innovation Center(No.20200627215553988)the Key projects for core technology research of Dongguan(No.2019622119003)。
文摘The energy density of commercial lithium(Li)ion batteries with graphite anode is reaching the limit.It is believed that directly utilizing Li metal as anode without a host could enhance the battery’s energy density to the maximum extent.However,the poor reversibility and infinite volume change of Li metal hinder the realistic implementation of Li metal in battery community.Herein,a commercially viable hybrid Li-ion/metal battery is realized by a coordinated strategy of symbiotic anode and prelithiated cathode.To be specific,a scalable template-removal method is developed to fabricate the porous graphite layer(PGL),which acts as a symbiotic host for Li ion intercalation and subsequent Li metal deposition due to the enhanced lithiophilicity and sufficient ion-conducting pathways.A continuous dissolution-deintercalation mechanism during delithiation process further ensures the elimination of dead Li.As a result,when the excess plating Li reaches 30%,the PGL could deliver an ultrahigh average Coulombic efficiency of 99.5% for 180 cycles with a capacity of 2.48 m Ah cm^(-2) in traditional carbonate electrolyte.Meanwhile,an air-stable recrystallized lithium oxalate with high specific capacity(514.3 m Ah g^(-1))and moderate operating potential(4.7-5.0 V)is introduced as a sacrificial cathode to compensate the initial loss and provide Li source for subsequent cycles.Based on the prelithiated cathode and initial Li-free symbiotic anode,under a practical-level3 m Ah capacity,the assembled hybrid Li-ion/metal full cell with a P/N ratio(capacity ratio of Li Ni_(0.8)Co_(0.1)Mn_(0.1)O_(2) to graphite)of 1.3exhibits significantly improved capacity retention after 300 cycles,indicating its great potential for high-energy-density Li batteries.
基金supported by the National Key Basic Research Program of China (No.2014CB932400)Joint Fund of the National Natural Science Foundation of China (No.U1401243)+2 种基金National Natural Science Foundation of China (No.51232005)Shenzhen Technical Plan Project (No.JCYJ20150529164918735,CYJ20170412170911187,KQJSCX20160226191136)Guangdong Technical Plan Project (No.2015TX01N011)。
文摘In this work, the electrochemical performance of LiNi0.8Co0.1Mn0.1O2(NCM811) has been investigated after cycling with various upper cutoff voltages. Noteworthily, electrochemical impedance of NCM811 declined with the increasing cycle number to high voltages. It was found that the decline of charge transfer impedance could be related to the structural and compositional change of cathode electrolyte interphase(CEI) of NCM811 when charging to high voltages, based on the characterization of electrochemical impedance spectroscopy(EIS), X-ray photoelectron spectroscopy(XPS) and transmission electron microscopy(TEM). The corresponding mechanism has also been proposed in this study. Specifically, due to the increasing roughness of cathode surface, the bottom of CEI film and cubic phase on cathode surface form a transition region mainly at high voltages, leading to the nonobvious boundary. This newly formed transition region at high voltages could promote the Li ion diffusion from electrolyte to cathode, then reducing charge transfer impedance. Additionally, the decrease of Li F on the surface of the cathode could also make a contribution to lower the interface impedance. This study delivers a different evolution of CEI on NCM811, and the impact of CEI evolution on electrochemical performance when charging to a high voltage.
基金supported by the National Natural Science Youth Fund of China(52302247)the Natural Youth Science Foundation of Hunan Province(2022JJ40070)。
文摘Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.
基金financial support from the National Natural Science Foundation of China(Nos.52261160384 and 52072208)the Project of Department of Education of Guangdong Province(No.2022ZDZX3018)+2 种基金the Natural Science Foundation of Guangdong(No.2023A1515010020)the Innovation and Technology Fund(No.ITS-325-22FP)the Shenzhen Science and Technology Program(No.KJZD20230923114107014)。
文摘Rechargeable lithium batteries with high-capacity cathodes/anodes promise high energy densities for nextgeneration electrochemical energy storage.However,the associated limitations at various scales greatly hinder their practical applications.Functional gradient material(FGM)design endows the electrode materials with property gradient,thus providing great opportunities to address the kinetics and stability obstacles.To date,still no review or perspective has covered recent advancements in gradient design at multiple scales for boosting lithium battery performances.To fill this void,this work provides a timely and comprehensive overview of this exciting and sustainable research field.We begin by overviewing the fundamental features of FGM and the rationales of gradient design for improved electrochemical performance.Then,we comprehensively review FGM design for rechargeable lithium batteries at various scales,including natural or artificial solid electrolyte interphase(SEI)at the nanoscale,micrometer-scale electrode particles,and macroscale electrode films.The link between gradient structure design and improved electrochemical performance is particularly highlighted.The most recent research into constructing novel functional gradients,such as valence and temperature gradients,has also been explored.Finally,we discussed the current constraints and future scope of FGM in rechargeable lithium batteries,aiming to inspire the development of novel FGM for next-generation high-performance lithium batteries.
基金the support from the Key-Area Research and Development Program of Guangdong Province (2020B090919003)the Yunnan Major Scientific and Technological Projects (202202AG050003)+4 种基金the Natural Science Foundation of China (22202078, 51904135,52162030)the Department of Education of Guangdong Province(2020KQNCX082)the Applied Basic Research Foundation of Yunnan Province (202103AA080019)the National Key R&D Program of China (2018YFB01040)the support of the supported by the Testing Technology Center of Materials and Devices of Tsinghua Shenzhen International Graduate School (SIGS)
文摘Advanced electrolyte engineering is an important strategy for developing high-efficacy lithium(Li)metal batteries(LMBs).Unfortunately,the current electrolytes limit the scope for creating batteries that perform well over temperature ranges.Here,we present a new electrolyte design that uses fluorosulfonyl carboxylate as a non-solvating solvent to form difluoroxalate borate(DFOB-)anion-rich solvation sheath,to realize high-performance working of temperature-tolerant LMBs.With this optimized electrolyte,favorable SEI and CEI chemistries on Li metal anode and nickel-rich cathode are achieved,respectively,leading to fast Li^(+)transfer kinetics,dendrite-free Li deposition and suppressed electrolyte deterioration.Therefore,Li||LiNi_(0.80)Co_(0.15)Al_(0.05)O_(2)batteries with a thin Li foil(50μm)show a long-term cycling lifespan over 400 cycles at 1C and a superior capacity retention of 90%after 200 cycles at 0.5C under 25℃.Moreover,this electrolyte extends the operating temperature from-10 to 30℃and significantly improve the capacity retention and Coulombic efficiency of batteries are improved at high temperature(60℃).Fluorosulfonyl carboxylates thus have considerable potential for use in high-performance and allweather LMBs,which broadens the new exploring of electrolyte design.
基金supported by National Natural Science Foundation of China(Grant No.52100084)Shenzhen Natural Science Fund(the Stable Support Plan Program GXWD20201230155427003-20200824094017001).
文摘Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that is stable in ambient air with an average operating voltage of~3.8 V,demonstrating excellent cycling stability with a capacity retention of more than 92.7%after 500 cycles at 20 mA g^(-1) and good rate capability with 91.9%capacity utilization at 500 mA g^(-1) with respect to capacity at 5 mA g^(-1) between 2.0 and 4.0 V.When the upper cutoff voltage is increased to 4.4 V,P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) delivers a reversible capacity of 71.9 mAh g^(-1) and retains 91.8%of the capacity after 100 cycles at 20 mA g^(-1).The charge compensation during charge/discharge is mainly due to the redox couple of Ni^(2+)/Ni^(3+)in the host with a small amount of contribution from oxygen.The stable structure of the material without phase transformation and with small volume change during charge-discharge allows it to give excellent cycle performance especially when the upper cutoff voltage is not higher than 4.2 V.
