Cathode Electrolyte Interphase Research Articles

Engineering Stable Decomposition Products on Cathode Surfaces to Enable High Voltage All-Solid-State Batteries.

Sulfide solid electrolytes such as Li6PS5Cl hold high promise for solid state batteries due to their high ionic conductivity; however, their oxidation potential of ~2.5 V is not compatible with high voltage Ni-rich cathodes such as LiNixCoyMn1-x-yO2 (x≥0.8). Here, we devise an effective, conformal and thin coating on the cathode active material guided by density functional theory, which suppresses the oxidative decomposition of Li6PS5Cl as shown by experiment. The nanometric coating on nickel-rich NMC85 enabled capacity retention of 82% after 200 cycles (2.8-4.3 V vs Li+/Li) using Li6PS5Cl as the solid electrolyte. In comparison, cells with an uncoated CAM only displayed 56% capacity retention. The coated-NCM85 cells also demonstrate much better rate performance and higher capacity. The enhanced performance is due to the formation of a stable amorphous cathode-electrolyte interphase accruing from the decomposition products of the LiPO2F2 precursor (as predicted by DFT), which protect the sulfide electrolyte from oxidation. The coating fabricated in this cost-effective process showed superior performance to state-of-the-art coatings such as LiNbO3. This work highlights the importance of rationally designing stable coating materials based on their potential decomposition products and confirms the suitability of a low-cost and conformal coating to enable sulfide electrolyte-based all-solid-state batteries.

Ultrafast Tailoring Amorphous Zn0.25V2O5 with Precision‐Engineered Artificial Atomic‐Layer 1T′‐MoS2 Cathode Electrolyte Interphase for Advanced Aqueous Zinc‐Ion Batteries

AbstractVanadium (V)‐based oxides as cathode materials for aqueous zinc‐ion batteries (AZIBs) still encounter challenges such as sluggish Zn2+ diffusion kinetics and V‐dissolution, thus leading to severe capacity fading and limited life span. Here, we designed an ultrafast and facile colloidal chemical synthesis strategy based on crystalline Zn0.25V2O5 (c‐ZVO) to successfully prepare a‐ZVO@MoS2 core@shell heterostructures, where atomic‐layer MoS2 uniformly coats on the surface of amorphous a‐ZVO. The tailored amorphous structure of a‐ZVO provides more isotropic pathways and active sites for Zn2+, thus significantly enhancing the Zn2+ diffusion kinetics during charge–discharge processes. Meanwhile, as an efficient artificial cathode electrolyte interphase, the precision‐engineered atomic‐layer MoS2 with semi‐metallic 1T′ phase not only contributes to improved electron transport but also effectively inhibits the V‐dissolution of a‐ZVO. Therefore, the prepared a‐ZVO@MoS2 and conceptually validated a‐V2O5@MoS2 derived from commercial c‐V2O5 exhibit excellent cycling stability at an ultralow current density (0.05 A g−1) while maintaining good rate capability and capacity retention. This research achievement provides a new effective strategy for various amorphous cathode designs for AZIBs with superior performance.

Challenges and Modification Strategies on High-Voltage Layered Oxide Cathode for Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) have attracted great attention due to their advantages on resource abundance, cost and safety. Layered oxide cathodes (LOCs) of SIBs possess high theoretical capacity, facile synthesis and low cost, and are promising candidates for large scale energy storage application. Increasing operating voltage is an effective strategy to achieve higher specific capacity and also high energy density of SIBs. However, at high operating voltages, LOCs will undergo a series of phase transitions in bulk phase, leading to huge change of volume and layer spacings accompanied by severe lattice stress and cracking formation. Degeneration of surface also occurs between LOCs and electrolytes, resulting in sustained growth of cathode electrolyte interphase (CEI) and release of O2 and CO2. These induce structural destruction and electrochemical performance degradation in high voltage regions. Recently, many strategies have been proposed to improve electrochemical performance of LOCs under high voltages, including bulk element doping, structural design, surface coating and gradient doping. This review describes pivotal challenges and occurrence mechanisms at high voltages, and summarizes strategies to improve stability of bulk and surface. Viewpoints will be provided to promote development of high energy density SIBs.

Ether-Modified Nonflammable Phosphate Enabling Anion-Rich Electrolyte for High-Voltage Lithium Metal Batteries.

Phosphate-based localized high-concentration electrolytes (LHCE) feature high flame retardant and satisfactory cathodic stability for lithium metal batteries. However, stable cycling of those electrolytes at ultra-high upper cut-off voltages for long-term stability remains challenging. Herein, an ether-modified phosphate, diethyl (2-methoxy ethoxy) methylphosphonate (DMEP), is designed for high-voltage applications. The ether modification enhances the stability of the Li+-DMEP-FSI- coordination structure, promoting the formation of cation-anion aggregates (AGG) dominated solvation structure, which favors the generation of LiF-rich cathode electrolyte interphase layers compared to triethyl phosphate (TEP)-based LHCE. Consequently, cathode degradation, including transition-metal dissolution and electrode cracking, is well-suppressed. The LiNi0.8Co0.1Mn0.1O2 (NCM811)||Li full cells using DMEP-based LHCEs show more than 90.7% capacity retention at an ultrahigh upper cut-off voltage of 4.7 V after 100 cycles. Notably, DMEP-LHCE exhibits enhanced safety than that of TEP-LHCE, suggesting its versatility and potential for next-generation lithium metal batteries.

Modulating Interfacial Solvation via Ion Dipole Interactions for Low‐Temperature and High‐Voltage Lithium Batteries

Extending the stability of ether solvents is pivotal for developing low‐temperature and high‐voltage lithium batteries. Herein, we elucidate the oxidation behavior of tetrahydrofuran with ternary BF4‐, PF6‐ and difluoro(oxalato)borate anions and the evolution of interfacial solvation environment. Combined in‐situ analyses and computations illustrate that the ion dipole interactions and the subsequent formation of ether‐Li+‐anion complexes in electrolyte rearrange the oxidation order of solvated species, which enhances the electrochemical stability of ether solvent. Furthermore, preferential absorption of anions on the surface of high‐voltage cathode favors the formation of a solvent‐deficient electric double layer and an anti‐oxidation cathode electrolyte interphase, inhibiting the decomposition of tetrahydrofuran. Remarkably, the formulated electrolyte based on ternary anion and tetrahydrofuran solvent endows the LiNi0.8Co0.1Mn0.1O2 cathode with considerable rate capability of 5.0 C and high capacity retention of 93.12% after 200 cycles. At a charging voltage of 4.5 V, the Li||LiNi0.8Co0.1Mn0.1O2 cells deliver Coulombic efficiency above 99% at both 25 and ‐30 °C.

Modulating Interfacial Solvation via Ion Dipole Interactions for Low-Temperature and High-Voltage Lithium Batteries.

Extending the stability of ether solvents is pivotal for developing low-temperature and high-voltage lithium batteries. Herein, we elucidate the oxidation behavior of tetrahydrofuran with ternary BF4-, PF6- and difluoro(oxalato)borate anions and the evolution of interfacial solvation environment. Combined in-situ analyses and computations illustrate that the ion dipole interactions and the subsequent formation of ether-Li+-anion complexes in electrolyte rearrange the oxidation order of solvated species, which enhances the electrochemical stability of ether solvent. Furthermore, preferential absorption of anions on the surface of high-voltage cathode favors the formation of a solvent-deficient electric double layer and an anti-oxidation cathode electrolyte interphase, inhibiting the decomposition of tetrahydrofuran. Remarkably, the formulated electrolyte based on ternary anion and tetrahydrofuran solvent endows the LiNi0.8Co0.1Mn0.1O2 cathode with considerable rate capability of 5.0 C and high capacity retention of 93.12% after 200 cycles. At a charging voltage of 4.5 V, the Li||LiNi0.8Co0.1Mn0.1O2 cells deliver Coulombic efficiency above 99% at both 25 and -30 °C.

High-efficient sodium compensation enabled by dual-carbon coupling catalyst strategy for sodium-ion batteries

Sodium oxalate (Na2C2O4), a green, cost-effective, and high-capacity additive candidate, suffers from a decomposition voltage that largely exceeds the cutoff voltage of currently common layered oxides and polyanionic compounds, limiting its availability. This work constructs a composite structure of carbon-coated Na2C2O4 coupled with a catalyst-loaded Ketjen black (NCO@C@MMNKB) using a low-temperature carbon-coated assisted ball milling technique. The results show that the decomposition potential of Na2C2O4 is significantly reduce from 4.42 to 3.91 V. Meanwhile, correspondingly the full cell energy density is enhanced from 135.0 to 236.4 Wh Kg−1. Further investigations show that the by-products of the sodium compensation additive exhibit different “gas effects” on the formation of the cathode and anode solid electrolyte interphase (CEI and SEI) films. This provides a practical thought to promote similar additives towards practicality to improve the overall performance of SIBs.

Electrolyte additive strategy to eliminate hydrofluoric acid and construct robust cathode electrolyte interphase for 4.6 V Li||LiCoO2 batteries

The high voltage of Li||LiCoO2 battery can increase the energy density. However, the cycling performance associated with cathode structural stability remains challenging. To address this question, we proposed an electrolyte strategy for improving the performance of 4.6 V Li||LiCoO2 battery by using trimethylsilyl isocyanate (TMIS) as electrolyte additive. The trimethylsilyl group of trimethylsilyl isocyanate can trap HF while the isocyanate group brings polyamide components to the CEI and the SEI. By the synergistic action, the Co3+ dissolution problem of the LiCoO2 cathode was effectively curbed. Furthermore, TMIS regulates the construction of anion-dominated LiF-rich SEI by influencing the solvation structure of Li+. As expected, the 4.6 V Li||LiCoO2 battery with trimethylsilyl isocyanate retains 77.9% initial capacity after 200 cycles at 0.5 C.

Comparative Study of High Voltage Spinel∥Lithium Titanate Lithium‐ion Batteries in Ethylene Carbonate Free Electrolytes

AbstractA persistent obstacle towards the realization of high voltage cathodes is electrolyte instability where oxidation and transition metal dissolution manifest in rapid capacity failure with both issues connected to the presence of ethylene carbonate in the electrolyte. Here, alternative electrolyte co‐solvents are investigated and compared, where the cyclic carbonate is replaced with sulfones ethyl methyl sulfone (EMS) and tetra methylene sulfone (TMS) and fluoroethylene carbonate (FEC). The best full cell performance was observed for cells cycled in a FEC/EMC (3/7) and FEC/EMC (1/1) electrolytes which exhibited 84–85 % capacity retention after 500 cycles. TMS/EMC (3/7), was determined to be the best performing sulfone electrolyte and maintained 71 % capacity after 500 cycles. Post‐mortem XPS analysis indicated different film forming mechanisms for the respective co‐solvent. A thicker cathode electrolyte interphase (CEI) on the LNMO was observed for the FEC containing electrolytes (relative to when TMS was used as the co‐solvent) indicating more effective passivation of the reactive cathode surface which correlated well with the enhanced cycling stability observed. For LTO, more evidence of transition metal migration and a thicker solid electrolyte interphase (SEI) layer was observed for the sulfone electrolyte suggesting more parasitic anode‐electrolyte interactions and an inability to mitigate Mn2+/Ni2+ crosstalk.

Dual Function of Hydrogen Bond and CEI to Enhanced Lithium-Ion Battery Performance.

The stability of the commercial electrolyte is linked to the internal solvent molecule, particularly in enhancing the stability of these molecules. Hereby, we introduce a dual function strategy involving hydrogen bond induced solvent molecules and the in situ fabrication cathode-electrolyte interphase (CEI) to address this issue. The additive N-(4-(2,5-dioxo-4-oxazolidinyl)butyl)-2,2,2-trifluoroacetamide (DOTFA), with its oxazolidinyl and trifluoroacetamide functional units, establishes hydrogen bonds with the solvent, forming CEI films on the cathode surface that enhance the antioxidation ability of the electrolyte. These hydrogen bonds contribute to enhancing the high-pressure structural stability of the solvent molecule. Additionally, the uniform and robust in situ constructed CEI films act as a shield, protecting the cathode from various side reactions and enhancing interface compatibility. By incorporation of the DOTFA additive in the electrolyte, lithium-ion batteries with NCM811 cathodes exhibit excellent cycling performance. The work highlights the significance of dual function in solvent molecules and provides an effective method for enhancing the antioxidation ability of the electrolyte.

Transforming Zinc-Ion Batteries with DTPA-Na: A Synergistic SEI and CEI Engineering Approach for Exceptional Cycling Stability and Self-Discharge Inhibition.

Aqueous zinc-ion batteries (ZIBs) hold immense potential for large-scale energy storage, but their practical implementation faces significant challenges related to the zinc anode, including dendrite formation, corrosion, and hydrogen evolution. This study addresses these challenges by introducing diethylenetriamine pentaacetate sodium salt (DTPA-Na) as a novel electrolyte additive. DTPA-Na exhibits a unique dual functionality, enabling the formation of a robust, multi-layered solid electrolyte interphase (SEI) on the zinc anode and a stable cathode electrolyte interphase (CEI) on the MnOOH cathode. The engineered SEI effectively suppresses interfacial side reactions, facilitates uniform zinc deposition, and mitigates dendrite growth, while the CEI inhibits MnOOH dissolution and detrimental cathode side reactions. This synergistic SEI/CEI engineering approach significantly enhances ZIB performance, achieving remarkable cycling stability and self-discharge inhibition, as evidenced by the extended lifespan of Zn||Zn symmetrical cells (4400 hours at 0.5 mA/cm2) and the exceptional capacity retention of Zn||MnOOH full cells after prolonged rest (98.61 % after 720 hours).

Solvation Regulation via Hydrogen Bonding to Mitigate Al Current Collector Corrosion for High‐Voltage Li‐Ion Batteries

AbstractThe exceptional thermal stability and conductivity of lithium bis(fluorosulfonyl)imide (LiFSI) have made it a preferred salt for lithium‐ion batteries (LIBs). However, the corrosion of aluminum (Al) current collectors by LiFSI at low potentials (3.8 V vs Li/Li+) poses a persistent challenge, hindering the application of LiFSI in 4 V‐class LIBs. Herein, 2,2,2‐trifluoroethyl methanesulfonate (TFMS) is proposed as a versatile co‐solvent to address the issue of Al current collector corrosion. It is demonstrated that incorporating TFMS into a conventional LiFSI‐based carbonate electrolyte can precisely tailor the Li+ solvation structure by hydrogen bonding interactions with dimethyl carbonate (DMC) solvent. This weakens the coordination between DMC and Li+ while increasing the participation of FSI− anions in the primary solvation shell, effectively suppressing the Al current collector caused by free FSI− anions attacking. Furthermore, TFMS and FSI− synergically induce the formation of an inorganic‐rich and compact cathode electrolyte interphase, significantly avoiding undesired side reactions. As a result, the TFMS‐electrolyte enables 1.2 Ah‐graphite||NCM811 (LiNi0.8Co0.1Mn0.1O2) pouch‐cells to achieve 89.9% capacity retention with high average Coulombic efficiency of >99.9% for 200 cycles at a cut‐off voltage of 4.4 V, opening up opportunities for the development of advanced high‐voltage LIBs.

Conformational isomerism breaks the electrolyte solubility limit and stabilizes 4.9 V Ni-rich layered cathodes

By simply increasing the concentration of electrolytes, both aqueous and non-aqueous batteries deliver technical superiority in various properties such as high-voltage operation, electrode stability and safety performance. However, the development of this strategy has encountered a bottleneck due to the limitation of the intrinsic solubility, and its comprehensive performance has reached its limit. Here we demonstrate that the conformational isomerism of the solvent would significantly affect the solubility of electrolytes. By transforming the configuration of solvent from cis-cis to cis-trans upon thermal triggering, we successfully break the solubility limit, and a beyond concentrated electrolyte with the lowest solvent-to-salt molar ratio of 0.70 is constructed. Transitions between cis-cis and cis-trans conformers are observed through Nuclear Magnetic Resonance (NMR) testing. The electrolyte consists entirely of anion-mediated solvation structures and promotes the formation of robust inorganic-dominated cathode electrolyte interphase. As a result, it enables stable cycling of 4.9 V-class LiNi0.8Co0.1Mn0.1O2 positive electrodes. Moreover, a high capacity of 151.2 mAh g−1 can be maintained after 1000 cycles at cut-off voltage of 4.8 V. This work provides a chemical pathway to build new concept electrolytes working under harsh conditions.

Catalytic Strategies Enabled Rapid Formation of Homogeneous and Mechanically Robust Inorganic‐Rich Cathode Electrolyte Interface for High‐Rate and High‐Stability Lithium‐Ion Batteries

AbstractLithium iron phosphate (LFP) cathode is renowned for high thermal stability and safety, making them a popular choice for lithium‐ion batteries. Nevertheless, on one hand, the fast charge/discharge capability is fundamentally constrained by low electrical conductivity and anisotropic nature of sluggish lithium ion (Li+) diffusion. On the other hand, the interface and internal structural degradation occurs when subjected to high‐rate condition. Herein, a multifunctional boron‐doping graphene/lithium carbonate (BG/LCO) nanointerfacial layer on surface of commercial LiFePO4 particles is designed, in which the BG layer catalyzes the rapid reaction of Li2CO3‐LiPF6 for homogeneous and mechanically robust inorganic LiF‐rich structure across the cathode‐electrolyte interphase (CEI), forms a conductive network to significantly enhance both electron and Li+ transport, and strengthens the FeO bonding to minimize both Fe loss and the formation of Fe‐Li antisite defects. Correspondingly, the modified LFP cathode achieves a high capability of 113.2 mAh g−1 at 10 C and extraordinary cyclic stability with 88.0% capacity retention over 1000 cycles as compared to the pristine LFP cathode with a capacity of only 94.0 mAh g−1 and 64.6% capacity retention. It also exhibits great enhancements of 20.1% and 3.7% at higher‐rate condition (room temperature/15 C) and the low temperature condition (−10 °C/1 C), respectively.

Sulfolane-Based Flame-Retardant Electrolyte for High-Voltage Sodium-Ion Batteries

HighlightsNaTFSI/SUL:OTE:FEC facilitates the formation of S, N-rich, dense and robust cathode–electrolyte interphase on NaNMF cathode, which improves the cycling stability under high voltage.By utilizing NaTFSI/SUL:OTE:FEC, the Na||NaNMF batteries achieved an impressive retention of 81.15% after 400 cycles at 2 C with the cutoff voltage of 4.2 V.The study offers a reference for the utilization of sulfolane-based electrolytes in sodium-ion batteries (SIBs), while the nonflammability of the NaTFSI/SUL:OTE:FEC enhances the safety of SIBs.

Revealing the Dynamic Evolution of Electrolyte Configuration on the Cathode‐Electrolyte Interface by Visualizing (De) Solvation Processes

AbstractElectrolyte engineering is crucial for improving cathode electrolyte interphase (CEI) to enhance the performance of lithium‐ion batteries, especially at high charging cut‐off voltages. However, typical electrolyte modification strategies always focus on the solvation structure in the bulk region, but consistently neglect the dynamic evolution of electrolyte solvation configuration at the cathode‐electrolyte interface, which directly influences the CEI construction. Herein, we reveal an anti‐synergy effect between Li+‐solvation and interfacial electric field by visualizing the dynamic evolution of electrolyte solvation configuration at the cathode‐electrolyte interface, which determines the concentration of interfacial solvated‐Li+. The Li+ solvation in the charging process facilitates the construction of a concentrated (Li+‐solvent/anion‐rich) interface and anion‐derived CEI, while the repulsive force derived from interfacial electric field induces the formation of a diluted (solvent‐rich) interface and solvent‐derived CEI. Modifying the electrochemical protocols and electrolyte formulation, we regulate the “inflection voltage” arising from the anti‐synergy effect and prolong the lifetime of the concentrated interface, which further improves the functionality of CEI architecture.

Promoting Interfacial Reaction via Quantifying NMC811 CEI Evolution and Li+ Desolvation Using Single‐Particle Electrochemical Methods

AbstractPromoting interfacial kinetics of high‐nickel LiNi0.8Mn0.1Co0.1O2 (NMC811) is a critical strategy for enhancing rate capability of lithium‐ion batteries (LIBs). At the solid‐liquid interface of positive electrode, charge transfer across the cathode‐electrolyte interphase (CEI) is responsible for the interfacial redox reaction, which is dominated by desolvation process of Li+ and NMC811 CEI evolution. Since these two processes are significantly impacted by the solvation effect of electrolytes, herein single‐particle Raman spectroscopy and single‐particle probes are established to quantitatively study the influences of solvation effect on CEI evolution and desolvation process of Li+, respectively. Owing to oxidation of the unstable free cyclic carbonate ester from dissociation of solvation structure, the CEI is found to grow thicker during discharge process. Due to the decreased concentration of cyclic carbonate in the solvation structure, the desolvation process of Li+ in the ethyl methyl carbonate‐ethylene carbonate electrolyte can be reduced by 11.8% compared to that in the dimethyl carbonate‐ethylene carbonate electrolyte. With the presence of ethyl methyl carbonate‐ethylene carbonate electrolyte, thinner CEI and easier desolvation process of Li+ can be simultaneously achieved on the NMC811 surface. Accordingly, its corresponding LIBs deliver the highest specific capacity ≈138.8 mAh g−1 at 5C among the LIBs with the other commonly used electrolytes.

Dual-Anionic Coordination Manipulation Induces Phosphorus and Boron-Rich Gradient Interphase Towards Stable and Safe Sodium Metal Batteries.

High-voltage sodium metal batteries (SMBs) present a viable pathway towards high-energy-density sodium-based batteries due to the competitive cost advantage and abundant supply of sodium resources. However, they still suffer from severe capacity decay induced by the notorious decomposition of the electrolyte under high voltage and unstable cathode/electrolyte interphase (CEI). In addition, the high reactivity of Na metal and flammable electrolytes push SMBs to their safety limits. Herein, a special dual-anion aggregated Na+ solvation structure is designed in a nonflammable trimethyl phosphate-based localized high-concentration electrolyte, and a gradient CEI enriched with phosphorus and boron compounds is formed on the cathode. This thin and stable interphase effectively suppresses the parasitic reaction, improves the interfacial stability of the cathode, and facilitates Na+ transport through the interface by the synergistic effect of multi-components, thus optimizing the cycling stability and safety of SMBs. The Na0.95Ni0.4Fe0.15Mn0.3Ti0.15O2//Na batteries employing such electrolyte provide a discharge capacity of 167.5 mA h g-1 and high retention in the capacity of 85.2% after 800 cycles at 1 C. This approach offers a general strategy for the design of flame-retardant high-voltage electrolytes and the practical application of SMBs.

Understanding the improved performances of Lithium–Sulfur batteries containing oxidized microporous carbon with an affinity-controlled interphase as a sulfur host

Li–S batteries (LSBs) based on the solid-phase conversion reaction that contain microporous carbon (MC) materials as their S hosts exhibit high cycling stabilities. Oxidized MC with O-containing functional groups increases the capacity of LSBs and lowers their internal resistance. Although these polar functional groups should improve the electrolyte affinities of electrode materials, their effects on the MC–S cathode/electrolyte interface have not yet been clarified. Herein, we report the affinity between the MC–S cathode and electrolyte. Contrary to conventional wisdom, the O-containing functional groups form affinity-controlled interphases on the MC–S cathodes, alleviating electrolyte decomposition and the formation of a cathode–electrolyte interphase during LSB cycling. This lowers the internal resistance of the LSB by facilitating unhindered Li-ion conduction, which stabilizes cycling at a low electrolyte [μL]/S [mg] ratio of 2.0, with an improved capacity (from 6.58 to 309.4 mAh g−1) in the second cycle. Thus, the use of an affinity-controlled interphase should improve the energy densities of LSBs and other energy storage devices.

Densification of Cathode/Electrolyte Interphase to Enhance Reversibility of LiCoO2 at 4.65V.

For LiCoO2 (LCO) operated beyond 4.55V (vs Li/Li+), it usually suffers from severe surface degradation. Constructing a robust cathode/electrolyte interphase (CEI) is effective to alleviate the above issues, however, the correlated mechanisms still remain vague. Herein, a progressively reinforced CEI is realized via constructing Zr─O deposits (ZrO2 and Li2ZrO3) on LCO surface (i.e., Z-LCO). Upon cycle, these Zr─O deposits can promote the decomposition of LiPF6, and progressively convert to the highly dispersed Zr─O─F species. In particular, the chemical reaction between LiF and Zr─O─F species further leads to the densification of CEI, which greatly reinforces its toughness and conductivity. Combining the robust CEI and thin surface rock-salt layer of Z-LCO, several benefits are achieved, including stabilizing the surface lattice oxygen, facilitating the interface Li+ transport kinetics, and enhancing the reversibility of O3/H1-3 phase transition, etc. As a result, the Z-LCO||Li cells exhibit a high capacity retention of 84.2% after 1000 cycles in 3-4.65V, 80.9% after 1500 cycles in 3-4.6V, and a high rate capacity of 160mAhg-1 at 16 C (1 C=200mAg-1). This work provides a new insight for developing advanced LCO cathodes.