Irreversible Phase Transition Research Articles

Regulating Surface Oxygen Activity by Perovskite-Coating-Stabilized Ultrahigh-Nickel Layered Oxide Cathodes.

Ultrahigh-Ni layered oxides are proposed as promising cathodes to fulfill the range demand of electric vehicles; yet, they are still haunted by compromised cyclability and thermal robustness. State-of-the-art surface coating has been applied to solve the instability via blocking the physical contact between the electrolyte and the highly active Ni4+ ions on the cathode surface, but it falls short in handling the chemo-physical mobility of the oxidized lattice oxygen ions in the cathode. Herein, a direct regulation strategy is proposed to accommodate the highly active anionic redox within the solid phase. By leveraging the stable oxygen vacancies/interstitials in a lithium and oxygen dual-ion conductor (layered perovskite La4 NiLiO8 ) coating layer, the reactivity of the surface lattice oxygen ion is dramatically restrained. As a result, the oxygen release from the lattice is suppressed, as well as the undesired irreversible phase transition and intergranular mechanical cracking. Meanwhile, the introduced dual-ion conductor can also facilitate lithium-ion diffusion kinetics and electronic conductivity on the particle surface. This work demonstrates that accommodating the anionic redox chemistry by dual-ion conductors is an effective strategy for capacity versus stability juggling of the high-energy cathodes.

Electrolyte regulating and interface engineering for high voltage LiCoO2 lithium metal batteries

To achieve higher energy density of lithium ion batteries (LIBs), researchers are developing a new generation of high-voltage (≥4.5 V) LiCoO2 (LCO). Increasing the voltage is accompanied by the decomposition of the electrolyte, successive irreversible phase transitions, and dissolution of transition metals, etc., which are largely benefit from detrimental cathode-electrolyte interface reactions. Here, we construct a stable N, S-rich electrode/electrolyte interphase on both Li anode as well as LCO cathode to solve the above problems through the electrolyte design with the dual additives of acrylonitrile and phenyl vinyl sulfone. Specifically, the uniform N, S-rich cathode/electrolyte interphase (CEI) separates the electrolyte and LCO, and reduces the catalytic decomposition of the electrolyte by Co4+. Moreover, phenyl vinyl sulfone has an excellent compatibility with the Li metal anode due to the in-situ formed LiF-rich solid electrolyte interphase (SEI). With the modification of dual-additives, the LCO lithium metal battery exhibits high-capacity retention about 80 % over 1000 cycles at upper cut-off voltage of 4.5 V and 76 % over 300 cycles at 4.6 V.

Double sites doping local chemistry Adjustment: A Multiple-Layer oriented P2-Type cathode with Long-life and Water/Air stability for sodium ion batteries

P2-type Ni/Mn layered oxides have attracted intensive interest as a kind of promising cathode materials because of their high specific capacities and unique 2D Na+ diffusion path. However, the poor stability and irreversible phase transition at high voltage during charge and discharge process greatly hinders its practical applications. Herein, a novel double site substitution strategy is reported that large-sized K+ is riveted in the prismatic Na+ sites and Cu2+ is occupies in the transition metal sites. The K+ doping lead to the lattice expansion along c-axis, which facilitating sodium ions transport. In addition, the double sites substitution improves the stability of the materials exposed in air and water environments. A combined analysis of first-principles calculation simulation and experimental verification determining that larger interlayer spacing decreases the diffusion barrier of sodium ions. The as-prepared multiple-layer oriented P2-K0.05Na0.67Mn0.6Ni0.3Cu0.1O2 shows excellent rate performance, fast sodium ion transport ability and superior cycling performance with a high-capacity retention of 91.2 % at a high current density of 1 A g−1 after 1800th cycles. Therefore, this work provides a new insight for the design of stable and high-performance cathode materials for sodium ion batteries.

Unexplored Orthorhombic LiMn1–xTixO2 Cathode Materials with a Stable Atomic Site Occupancy and Phase Transition

Mn-rich orthorhombic (o)-LiMn1–xTixO2 with a stable oxygen/cation site occupancy and cycling-dependent phase transition is explored as a novel Co- and Ni-free cathode material for Li-ion rechargeable batteries. Typical o-LiMnO2 suffers from oxygen deficiency, cation mixing between Li and Mn, and monoclinic (m)-Li2MnO3 secondary phase with low conductivity. Together with these drawbacks, the gradual, irreversible phase transition from layered o-LiMnO2 into spinel-like cubic (c)-LixMnO2 (x ≈ 0.5) during repeated charge/discharge cycles degrades the cycling performance of o-LiMnO2 despite the activation of electroactive c-LixMnO2 (x ≈ 0.5). By contrast, o-LiMn1–xTixO2 consists of Ti-doped o-LiMnO2 and c-LiTiO2 as the primary and secondary phases, respectively. The presence of Ti–O bonds, stronger than the existing Mn–O bonds, improves the structural stability of Ti-doped o-LiMnO2 by reducing the imperfections of the oxygen/cation lattices (including Mn octahedral sites associated with the Jahn–Teller distortion) in Ti-doped o-LiMnO2 during the long-term synthesis under an inert atmosphere. In addition, the electrochemically inactive (>2 V vs Li+/Li) c-LiTiO2 phase with high conductivity serves as a pillar that suppresses the severe structural collapse of Ti-doped o-LiMnO2 through an abrupt phase/structural transition during cycling (2–4.5 V). As a result, o-LiMn1–xTixO2 with an optimal Ti content exhibits a higher maximum discharge capacity and superior cycling performance compared to the pristine o-LiMnO2.

Fundamental Understanding of the Effect of a Polyaniline Coating Layer on Cation Mixing and Chemical States of LiNi0.9Co0.085Mn0.015O2 for Li-Ion Batteries

A high nickel content of the cathode usually results in a large discharge capacity but causes structural collapse. Ni2+ ions move to the Li layer when Li+ ions are deintercalated during discharge, resulting in irreversible phase transition, cation mixing, dissolution of transition metal ions, and side reactions. A protective barrier is essential for maintaining the layered structures of cathode materials, even after several charge/discharge cycles of Li-ion batteries. Polyaniline (PANi) is an organic coating material with high conductivity and flexibility. PANi-coated cathodes have been widely reported for improving electrochemical performances. However, it is insufficient to prove the correlation between the PANi coating layer and structural stability through further analysis after an electrochemical test. Therefore, we focused on the structural stability and chemical states of the PANi-coated cathode after a cycle test by observing the morphology, lattice patterns, and chemical states of the surface. PANi-coated LiNi0.9Co0.085Mn0.015O2 (NCM; PANi@NCM) exhibited an initial discharge capacity of 221 mAh g–1 and a capacity retention of 81% after 50 cycles at 45 °C, which corresponded to an improved performance compared to pristine NCM. The cycled PANi@NCM showed an identical morphology to that of the cathode before the test. The R3̅m layered structure of PANi@NCM was maintained even after 50 cycles, as confirmed by transmission electron microscopy analysis with fast Fourier transform patterns and high-angle annular dark-field images. In addition, PANi@NCM maintains a thinner passivation layer (8 nm) compared with that of pristine NCM (27 nm). According to the X-ray photoelectron spectroscopy results, the surface chemical state of PANi@NCM showed that side reactions between the cathode and the electrolyte were suppressed during the cycle test. Therefore, it is demonstrated that the PANi coating layer prevents cation mixing and side reactions.

Magnesium doping improved characteristics of high voltage cycle of layered cathode of sodium ion battery

Driven by global demand for new energy, Li-ion batteries (LIBs) have developed rapidly due to their competitive performance. Although LIBs show the advantages of high capacity and good cycling stability, their disadvantages such as uneven distribution of lithium resources are gradually exposed. Therefore, with abundant reserves, Na-ion batteries (NIB) have become one of the most promising solutions to make up for the deficiency of Li-ion battery. The NIBs layered oxide cathodes have the most potential applications of cathode material due to their high specific capacity (167 mAh·g<sup>–1</sup> in 2.4–4.3 V) and simple synthesis method. However, improving the cycling stability of layered cathode materials is one of the keys to their large-scale industrialization. To develop high capacity and cycling stability cathode materials, the Mg<sup>2+</sup> is substituted for Ni<sup>2+</sup> in NaNi<sub>0.4</sub>Cu<sub>0.1</sub>Mn<sub>0.4</sub>Ti<sub>0.1</sub>O<sub>2</sub> (NCMT), thereby obtaining a NaNi<sub>0.35</sub>Mg<sub>0.05</sub>Cu<sub>0.1</sub>Mn<sub>0.4</sub>Ti<sub>0.1</sub>O<sub>2</sub> (NCMT-Mg) cathode material. The NCMT-Mg has a high reversible specific capacity of 165 mAh·g<sup>–1</sup> in a voltage window of 2.4–4.3 V. The reversible specific capacity of about 110 mAh·g<sup>–1</sup> at 0.1 C after 350 cycles with a capacity retention of 67.3% is about 13% higher than the counterpart of NCMT. The irreversible reaction is suppressed from P'3 phase to X phase for NCMT. The ex-XRD spectrometers further prove that the NCMT-Mg shows a P3 and X mixed phase after being initially charged to 4.3 V, but the NCMT shows an X phase. The irreversible phase transition is suppressed to increase the cycling stability. The inactive Mg<sup>2+</sup> replaces Ni<sup>2+</sup>, reducing the charge compensation and stabilizing the structure, the inactive Mg<sup>2+</sup> can activate the charge compensation of Ni<sup>2+</sup>/Cu<sup>2+</sup>. The electrochemical activity increases from 77% to 86%. The high capacity and excellent cycling stability prove that the NCMT-Mg structure remains intact after various current rates have been tested. The long cycling stability mechanism is further systematically studied by using various technologies. The present work will provide an important reference for developing high-performance Na-ion cathode materials.

Organic-inorganic haloargentate hybrids of [Me-dabco]Ag2X3 (X = I or Br) with halide ions manipulating the crystal structure, phase transition, and dielectric behavior.

Two haloargentate hybrids, [Me-dabco]Ag2X3 (Me-dabco = 1-methyl-1,4-diazabicyclo-[2.2.2]octan-1-ium, X = I (1) or Br (2)), with the same formula but different structures have been synthesized by a slow evaporation method and characterized by microanalysis, infrared spectroscopy, thermogravimetric, and powder X-ray diffraction techniques. Hybrid 1 consists of completely isolated [Ag4I6]2- clusters, while hybrid 2 exhibits a complicated one-dimensional (1D) chain structure formed by four different configurations of neutral chains and two dissimilar configurations of anionic chains. Hybrid 2 undergoes two reversible order-disorder phase transitions, while hybrid 1 displays one reversible and one irreversible structural phase transition. Both 1 and 2 displayed step-like dielectric anomalies in the vicinity of the phase transition temperature. The corresponding dielectric constants in the high dielectric states are approximately 13 and 6 times higher than those in the low dielectric states for 1 and 2, respectively. Interestingly, the subtle change of halides from I- to Br- significantly affects the aggregated structure of haloargentate, the phase transition, and dielectric behaviors, revealing the typical 'butterfly effect' with the ion radii of halides in these two haloargentate hybrids.

The improvement of the high voltage performance of LiCoO2 by coating LiTaO3via magnetron sputtering

We use magnetron sputtering technology to achieve a uniform LiTaO3 layer on the surface of LiCoO2 electrode. As an artificial CEI layer, this layer inhibits the irreversible phase transition of LiCoO2 crystal under high voltage.

Mg-Doped high voltage LiCoO2 for high performance lithium-ion batteries

Further increasing the voltage is the most efficient means of acquisition to obtain lithium cobalt oxide with high specific capacity, but the irreversible phase transition of LiCoO2 at high voltage leads to poor electrochemical performance. In this paper, a 4.6V high voltage stable lithium cobalt oxide cathode material was achieved by simple high temperature solid-phase synthesis method doped with different contents of Mg elements. Under the condition of Mg content of 0.02, the specific capacity of discharge is 222.7 mAh/g at 0.5C, and the capacity retention rate is 93% after 50 cycles of 1C, showing good electrochemical performance.

In Situ Inducing Spinel/Rock Salt Phases to Stabilize Ni-Rich Cathode via Sucrose Heat Treatment

Nickel-rich cathode materials have attracted widespread interest due to their high capacity; however, the structure is prone to degradation and collapse during cycling, resulting in poor stability performance and safety, hindering the development of high-nickel cathode materials. Here, we propose a straightforward method to consume oxygen on the surface of primary particles during the high-temperature calcination process of precursors, inducing the coupled rearrangement of surface cations, resulting in the in situ generation of a nano-sized mixed spinel/rock salt defect phase, which is confirmed by high-angle annular dark-field scanning transmission electron microscopy. LiNi 0.8 Co 0.1 Mn 0.1 O 2 modified with mixed phase not only can reduce side reactions with the electrolyte, resulting in fewer by-products such as LiF and Li 2 CO 3 , preventing the formation of excessively thick cathode–electrolyte interface layers, but also can avoid irreversible phase transitions and prevents lattice mismatches. As a result, the cycling performance has been improved to some extent, benefiting from structural stability. In addition, the special 3-dimensional structure of the spinel phase allows the material surface to expand ion transport channels and enhance multiplicative performance. Therefore, this study provides a new perspective on the modification of high-nickel materials and extends the application of nickel-rich materials.

Mean-field approximation for structural balance dynamics in heat bath.

A critical temperature for a complete signed graph of N agents where the time-dependent polarization of links tends towards the Heider (structural) balance is found analytically using the heat-bath approach and the mean-field approximation as T^{c}=(N-2)/a^{c}, where a^{c}≈1.71649. The result is in perfect agreement with numerical simulations starting from the paradise state where all links are positively polarized as well as with the estimation of this temperature received earlier with much more sophisticated methods. When heating the system, one observes a discontinuous and irreversible phase transition at T^{c} from a nearly balanced state when the mean link polarization is about x_{c}=0.796388 to a disordered and unbalanced state where the polarization vanishes. When the initial conditions for the polarization of links are random, then at low temperatures a balanced bipolar state of two mutually hostile cliques exists that decays towards the disorder and there is a discontinuous phase transition at a temperature T^{d} that is lower than T^{c}. The system phase diagram corresponds to the so-called fold catastrophe when a stable solution of the mean-field equationcollides with a separatrix, and as a result a hysteresislike loop is observed.

Long-Life Regenerated LiFePO4 from Spent Cathode by Elevating the d-Band Center of Fe.

A large amount of spent LiFePO4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li+ diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li+ migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d-band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen-doped carbon. The FeO bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d-band center. The Li+ diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10C with ≈80% capacity retention after 1000cycles.

Interlayer Modulation of Layered Transition Metal Compounds for Energy Storage.

Layered transition metal compounds are one of the most important electrode materials for high-performance electrochemical energy storage devices, such as batteries and supercapacitors. Charge storage in these materials can be achieved via intercalation of ions into the interlayer channels between the layer slabs. With the development of lithium-beyond batteries, larger carrier ions require optimized interlayer space for the unrestricted diffusion in the two-dimensional channels and effectively shielded electrostatic interaction between the slabs and interlayer ions. Therefore, interlayer modulation has become an efficient and promising approach to overcome the problems of sluggish kinetics, structural distortion, irreversible phase transition, dissolution of some transition metal elements, and air instability faced by these materials and thus enhance the overall electrochemical performance. In this review, we focus on the interlayer modulation of layered transition metal compounds for various batteries and supercapacitors. Merits of interlayer modulation on the charge storage procedures of charge transfer, ion diffusion, and structural transformation are first discussed, with emphasis on the state-of-art strategies of intercalation and doping with foreign species. Following the obtained insights, applications of modified layered electrode materials in various batteries and supercapacitors are summarized, which may guide the future development of high-performance and low-cost electrode materials for energy storage.

Operando Observation of Coupled Discontinuous-Continuous Transitions in Ion-Stabilized Intercalation Cathodes

Irreversible phase transition caused capacity fading has been considered as an obstacle for rechargeable batteries. An in-depth investigation of the irreversible phase transition is critical for understanding the reaction mechanism and developing advanced batteries. In this work, taking vanadium oxide and its alkali ion-stabilized intercalation compounds (A-V-O, A = Li, Na, K) as prototypes, utilizing operando characterizations, we discovered coupled discontinuous (interlayer)-continuous (intralayer) transitions in the stabilized multielectron intercalation cathodes. The highly ordered crystal of vanadium pentoxide irreversibly transfers to a disordered/amorphous structure after the first cycle, whereas A-V-O enables reversible discontinuous lattice transitions at the interlayer pathway for facilitating lithium diffusion. Among the A-V-O family, K-V-O, with the highest capacity retention, shows a coupled discontinuous-continuous transition, which exhibits a continuous transition and the minimum volume change at the V-O intralayer during lithium intercalation/deintercalation. These coupled discontinuous-continuous lattice transitions were captured for the first time in cathode materials. It implies that the suitable ion intercalation induced continuous intralayer transition inhibits the irreversible ion intercalation and phase transition.

Low‐Cost Zinc Substitution of Iron‐Based Prussian Blue Analogs as Long Lifespan Cathode Materials for Fast Charging Sodium‐Ion Batteries

AbstractIron‐based Prussian blue analogs (Fe‐PBAs) are extensively studied as promising cathode materials for rechargeable sodium‐ion batteries owing to their high theoretical capacity, low‐cost and facile synthesis method. However, Fe‐PBAs suffer poor cycle stability and low specific capacity due to the low crystallinity and irreversible phase transition during excess sodium‐ion storage. Herein, a modified co‐precipitation method to prepare highly crystallized PBAs is reported. By introducing an electrochemical inert element (Zn) to substitute the high‐spin Fe in the Fe‐PBAs (ZnFeHCF‐2), the depth of charge/discharge is rationally controlled to form a highly reversible phase transition process for sustainable sodium‐ion storage. Minor lattice distortion and highly reversible phase transition process of ZnFeHCF‐2 during the sodium‐ions insertion and extraction are proved by in‐situ tests, which have significantly impacted the cycling stability. The ZnFeHCF‐2 shows a remarkably enhanced cycling performance with capacity retention of 58.5% over 2000 cycles at 150 mA g−1 as well as superior rate performance up to 6000 mA g−1 (fast kinetics). Furthermore, the successful fabrication of the full cell on the as‐prepared cathode and commercial hard carbon anode demonstrates their potential as high‐performance electrode materials for large‐scale energy storage systems.

Effect of dopants and microstructure on the electrochemical cyclic stability of layered P2-type Na0.67MnO2 prepared by different chemical routes: An experimental and theoretical study

High specific capacity layered transition metal oxide, NaxMnO2 is considered a potential cathode for sodium-ion batteries (SIBs). However, its poor capacity retention due to irreversible phase transitions during sodium ion insertion/extraction remains a critical challenge for practical applications. Herein, we report Fe and Co co-doped P2-type Na0.67MnO2 cathode material prepared via different facile chemical routes to understand the effect of dopants and microstructure on its electrochemical cyclic stability. The Rietveld refinement analysis depicts an increase in lattice parameter c of Fe and Co doped materials as compared to parent material; thereby favouring sodium-ion storage (in turn enhancing and stabilizing specific capacity). XPS analysis confirms the presence of Mn in both 3+ and 4+ oxidation states; whereas Fe and Co in 3+ oxidation states occupy Mn3+ in Na0.67MnO2. Both experiment and ab initio magnetic calculations show a reduction in Mn3+ content after Fe and Co doping, reducing the tendency for Jahn-Teller distortion. This is concomitant with Fe and Co doping showing improved cyclic stability when cycled under similar conditions. At 0.1 C (where 1 C = 174 mAh g−1), Fe and Co-doped Na0.67MnO2 showed significant improvement with higher discharge specific capacities of 80 and 103 mAh g−1 even after 60th cycle when compared to 36 mAh g−1 after 25th cycle for the parent material Na0.67MnO2.

Synthesis of Fe3O4 nanocubes anchored in MgCo2O4 nanoneedle arrays for flexible all-solid-state asymmetric supercapacitor

The design of novel heterostructure with multifunctional characteristics is of great technical significance for the development of new energy storage devices. However, the lower conductivity of metal oxides and the accumulation caused by irreversible phase transition after multiple cycles are the main reasons for the low specific capacitance and cycle life. Herein, we synthesized bimetallic oxide MgCo2O4 nanoneedles with a spinel structure, and firmly anchored Fe3O4 nanocubes on MgCo2O4 nanoneedles by ion-exchange strategy. Thanks to the constructed heterostructure of nanoneedles/nanocubes, the introduction of Fe3O4 effectively improves the electron transport path in MgCo2O4 during repeated charging and discharging, and increases the effective activation sites involved in electron transfer. As a result, a higher specific capacitance of 1648 F g−1 at 1 A g−1 and an ultra-long cycle life of 78.6% capacitance retention after 6000 continuous charge/discharge cycles are obtained. A flexible all-solid-state asymmetric supercapcitor assembled with MgCo2O4-Fe3O4 as positive electrode and AC as negative electrode can deliver an ultra-high energy density of 78 Wh kg−1 and maximum power density of 1.2 kW kg−1, as well as extraordinary capacitive retention of 75.2% after 10,000 cycles. These excellent properties reveal the potential and application value of MgCo2O4-Fe3O4 in the development of high-performance supercapacitors.

Realization of a high voltage Ni rich layer LiNi0.5Co0.2Mn0.3O2 single crystalline cathode for LIBs by surface modification

Single crystalline ternary cathode material LiNi0.5Co0.2Mn0.3O2(NCM523) can operate at extremely high voltages and could offer exceptional energy density. The single crystal morphology is less easy to form the cracks and could express better structure stability compared to the polycrystalline counterpart. However, irreversible parasitic side reactions in the interface during cycling may lead to rapid electrochemical degradations. Herein, a simple chemical wet method that modifies the single-crystal NCM523 particles with Al2O3 coating is proposed. The coating layer can effectively suppress the phase transformation and irreversible phase transition on the NCM surface during cycling. Furthermore, the cladding layer can prevent the erosion of by-products such as HF. As a result, the Al2O3 modified NCM523 delivers a high specific capacity of 192.5mAh g−1, excellent cycling stability and rate capability. The capacity retention was 91.7% after 50 cycles even at ultra-high cut-off voltage of 4.7 V. This surface engineering strategy paves the way to promote the development of small size single crystal NCM523 materials for next generation LIBs.

New Ion Substitution Method to Enhance Electrochemical Reversibility of Co‐Rich Layered Materials for Li‐Ion Batteries

AbstractThe recent development of high‐energy LiCoO2 (LCO) and progress in the material recycling technology have brought Co‐based materials under the limelight, although their capacity still suffers from structural instability at highly delithiated states. Thus, in this study, a secondary doping ion substitution method is proposed to improve the electrochemical reversibility of LCO materials for Li‐ion batteries. To overcome the instability of LCO at highly delithiated states, Na ions are utilized as functional dopants to exert the pillar effect at the Li sites. In addition, Fe‐ion substitution (secondary dopant) is performed to provide thermodynamically stable surroundings for the Na‐ion doping. Density functional theory calculations reveal that the formation energy for the Na‐doped LCO is significantly reduced in the presence of Fe ions. Na and Fe doping improve the capacity retention as well as the average voltage decay at a cutoff voltage of 4.5 V. Furthermore, structural analysis indicates that the improved cycling stability results from the suppressed irreversible phase transition in the Na‐ and Fe‐doped LCO. This paper highlights the fabrication of high‐energy Co‐rich materials for high voltage operations, via a novel ion substitution method, indicating a new avenue for the manufacturing of layered cathode materials with a long cycle life.

Conversion of residual lithium into fast ionic conductor coating to achieve one-step double modification strategy in LiNi0.8Co0.15Al0.05O2

The application of Ni-rich ternary cathode materials is restricted by the irreversible phase transition and interfacial side reactions during long-term cycling. Herein, a LiTaO3 coating and Ta5+ doping strategy are simultaneously achieved by a simple solid-phase synthesis. The surface side-reaction and undesired phase transition of LiNi0.8Co0.15Al0.05O2 (NCA) are effectively restrained by this approach, which utilizes residual lithium to afford the coating. The NCA-LTO 3 (The modified NCA with a LiTaO3 coating content of 3 wt%) delivers a high reversible capacity of 168.04 at 5 C (140.56 mAh g−1 for NCA), revealing the enhanced rate capability. More importantly, the cycling life could be greatly maintained after 200 cycles with a significant capacity retention of 94.1% (61.2% for NCA) at 1 C. Mechanism analysis indicates that such improvement is ascribed to the coating of conductor LiTaO3 and doping Ta5+ greatly promoting the Li-ion diffusion and stabilizing the interface of NCA. The study proposes a highly convenient strategy for interfacial optimization of cathode materials toward assisting the large-scale production of high-performance NCA.