High Energy Density Research Articles

Stabilizing High-Voltage Performance of Nickel-Rich Cathodes via Facile Solvothermally Synthesized Niobium-Doped Strontium Titanate.

Ni-rich layered ternary cathodes are promising candidates thanks to their low toxic Co-content and high energy density (∼800 Wh/kg). However, a critical challenge in developing Ni-rich cathodes is to improve cyclic stability, especially under high voltage (>4.3 V), which directly affects the performance and lifespan of the battery. In this study, niobium-doped strontium titanate (Nb-STO) is successfully synthesized via a facile solvothermal method and used as a surface modification layer onto the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. The results exhibited that the Nb-STO modification significantly improved the cycling stability of the cathode material even under high-voltage (4.5 V) operational conditions. In particular, the best sample in our work could provide a high discharge capacity of ∼190 mAh/g after 100 cycles under 1 C with capacity retention over 84% in the voltage range of 3.0-4.5 V, superior to the pristine NCM811 (∼61%) and pure STO modified STO-811-600 (∼76%) samples under the same conditions. The improved electrochemical performance and stability of NCM811 under high voltage should be attributed to not only preventing the dissolution of the transition metals, further reducing the electrolyte's degradation by the end of charge, but also alleviating the internal resistance growth from uncontrollable cathode-electrolyte interface (CEI) evolution. These findings suggest that the as-synthesized STO with an optimized Nb-doping ratio could be a promising candidate for stabilizing Ni-rich cathode materials to facilitate the widespread commercialization of Ni-rich cathodes in modern LIBs.

A Comparative Study on Coupled Fluid–Thermal Field of a Large Nuclear Turbine Generator with Radial and Composited Radial–Axial–Radial Ventilation Systems

With the continuous growth of energy demand, the advantages of nuclear power, such as high energy density, low emissions, and cleanliness, are gradually highlighted. However, the increasing capacity of the turbine generator in nuclear power plants has led to greater losses and critical heating issues. Designing an effective cooling system plays an important role in improving the rotor’s heat dissipation ability, especially under the condition of limited rotor space. In this study, the cooling effects of the rotor using a radial straight-type cooling structure and a composited radial–axial–radial cooling structure are compared and analyzed for a 1555 MVA hydrogen-cooled nuclear turbine generator. Three-dimensional fluid thermal coupled models of the rotor with both cooling structures are established, and corresponding boundary conditions are provided. The models are solved using the finite volume method. The flow law of cooling hydrogen gas inside the rotor and the temperature distribution of various parts of the rotor are studied in detail. Compared with the radial straight-type cooling structure, adopting the composited radial–axial–radial cooling structure can reduce the average temperature of the rotor field windings by 4.5 °C. The research results provide a reference for the design and optimization of the rotor cooling system for large-capacity nuclear turbine generators.

Cation-polymerized artificial SEI layer modified Li metal applied in soft-matter polymer electrolyte.

Li metal batteries with polymer electrolyte are of great interest for next-generation batteries for high safety and high energy density. However, uneven deposition on the lithium metal surface can greatly affect battery life. Therefore, surface modification on the Li metal become necessary to achieve good performance. Herein, an artificial solid electrolyte interface (SEI) modified lithium metal anode is prepared using cation-polymerization process, as triggered by PF5 generated from CsPF6. As a result, the polarization voltage of Li||Li symmetric battery assembled with artificial SEI-modified Li metal anode was stable with a small over-potential of 25 mV after 3000 h at current density of 1.5 mA cm-2. Electrochemical performance of Li||NCM 622 (LiNi0.6Co0.2Mn0.2O2) full cell with soft-matter polymer electrolyte is significantly improved than bare Li-metal, the capacity retention is 75% after 120 cycles with N/P=3:1 at a cut-off voltage of 4.3 V. Our work has shed lights on the commercialization of Li metal battery with polymer electrolyte.

A Review of the Structure–Property Relationship of Nickel Phosphides in Hydrogen Production

Hydrogen, one of the most promising forms of new energy sources, due to its high energy density, low emissions, and potential to decarbonize various sectors, has attracted significant research attention. It is known that electrocatalytic hydrogen production is one of the most widely investigated research directions due to its high efficiency in the conversion of electricity to H2 gas. However, given the limited reserves and high cost of precious metals, the search for non-precious metal-based catalysts has been widely explored, for example, transition metal phosphides, oxides, and sulfides. Despite this interest, a detailed survey unveils that the surface and internal structures of the alternative catalysts, including their surface reconstruction, composition, and electronic structure, are poorly studied. As a result, a disconnection in the structure–property relationship severely hinders the rational design of efficient and reliable non-precious metal-based catalysts. In this review, by focusing on Ni5P4, a bifunctional catalyst for water splitting, we systematically summarize the material motifs pertaining to the different synthetic methods, surface characteristics, and hydrolysis properties. It is believed that a cascaded correlation may provide insights toward understanding the fundamental catalytic mechanism and design of robust alternative catalysts for hydrogen production.

Constructing an All Solid-state Flexible Lithium-Manganese Battery with High Performance

Abstract Due to a lack of portable flexible power supply, flexible electronic products can still not be applied in a large scale, particularly in the high energy density devices. To resolve this issue, flexible solid-state lithium batteries with a high safety, excellent mechanical property, and high energy densit，is proposed. In this paper, a flexible solid-state lithium-manganese battery is developed, which is assembled with a lithium cloth composite anode, a composite solid-state electrolyte poly (vinylidene fluoride)-hexafluoropropylene (PVDF-HFP)/Li6.4La3Ta0.6O12 (LLZTO), and a composite cathode (Fe ion-doped MnO2-carbon cloth). To improve the conductivity and stability of cathode, a mixture of conductive carbon black (Super P) and sodium alginate (SA) is employed. To ensure the high capacity and low price, the MnO2-based cathode is used.The obtained solid state batteries can deliver an initial capacity of 275.9 mAh g-1 at a current density of 1 C and a capacity retention of 57.9% (159.7 mAh g-1 ) after 1000 cycles. Also the produced flexible punch cell can light up the light-emitting diode(LED), and its capacity is 0.58 mAh cm-2 after 100 cycles at current density of 0.2 C.

Structural energy storage composites based on etching engineering Fe-doped Co MOF electrode toward high energy density supercapacitors

Metal organic frameworks (MOFs) have been used widely as cathode materials for supercapacitors because of their adjustable chemical composition, variable topological structures, and relatively simple synthesis methods. However, most MOFs are insulated and their metal organic ligand coordination bonds are not stable enough in electrolytes, which greatly limits the application of MOFs in supercapacitors. The synergistic effect between transition metal doped and chemical etching is of great significance for the preparation of high-performance MOF electrodes. This study introduces Fe into Co MOF prepared by co precipitation to optimize the electronic structure of Co, and then constructed e-Fe-doped Co MOF hierarchical structure through ammonia etching. The Co MOF achieves rapid electron exchange at the electrode electrolyte interface through this synergistic effect, improving conductivity, and increasing specific surface area, exposing more active sites, effectively enhancing the electrochemical activity of the electrode. Therefore, the e-Fe-doped Co MOF-4 h has a high specific capacity of 700 C g−1 at 1 A g−1 with a 90.08 % high-rate performance. The assembled e-Fe-doped Co MOF-4 h//N-doped WC ASC provides the energy density of 80 Wh kg−1 at a power density of 800 W kg−1 with a ∼88 % capacitance retention after 10000 cycles. These results provide ideas for utilizing synergistic effects to prepare high-energy density supercapacitors using MOF materials.

Hierarchical porous carbon with abundant N/O doping as an anode for zinc ion hybrid supercapacitors

Aqueous zinc-ion hybrid supercapacitors (ZISCs) known for their affordability, stability, and high energy density represent innovative energy storage devices. Porous carbon is usually used as the cathode material of ZISCs, and its structure significantly affects the dual performance of high power density and energy density of ZISCs. Herein, a one-pot carbonization strategy is proposed, eliminating the need for templates, additional heteroatom compounds, and activation processes. By precisely controlling the temperature to optimize the structure and electrochemical performance of carbon materials, we successfully synthesized hierarchical porous carbon materials (NOPC-800) with a high specific surface area of 1545.7 mg, featuring dual doping of 12.3 at% nitrogen and 13.35 at% oxygen. The self-doping of abundant nitrogen and oxygen atoms facilitates the chemical adsorption of ions and accelerates pseudocapacitive reaction kinetics. Leveraging these advantages, ZISCs were assembled using NOPC-800 as the positive electrode and zinc as the negative electrode, showcasing remarkable performance: a specific capacity of up to 121.9 mAh g, an energy density of 97.5 Wh kg, and a power density of up to 16000 W kg. Remarkably, NOPC-800 maintained an excellent capacity retention of 94.9% after 10,000 cycles at a current density of 10 A g. This research paves an innovative and feasible path for the design and advancement of novel heteroatom-rich carbon cathodes.

A [formula omitted]-radioisotope battery based on betavoltaic and beta-photovoltaic dual effects

Betavoltaic batteries with strontium sources are expected to achieve higher output power because of their high energy density and low self-absorption rate with the development of MEMS. However, the high energy of beta particles emitted from 90Sr/90Y can prone to radiation damage of the semiconductor. In order to exploit the high energy of beta particles emitted from 90Sr/90Y and to avoid radiation damage to the semiconductor, this paper presents a 90Sr/90Y-radioisotope battery based on betavoltaic (BV) and beta-photovoltaic (BPV) dual effects. In the work, the energy deposition of beta particles in LYSO:Ce and GaAs was simulated by Monte Carlo code, and thickness of the scintillator was determined. And the doping concentrations and junction depth of semiconductor were optimized based on the theoretical calculations to obtain the best output performance of device. When the thickness of LYSO:Ce is 0.158 cm, the output power density Pm of the optimized dual-effect battery is 0.61 μW/cm2. And the conversion efficiency of the device is 0.92%. At this time, the doping concentrations are Na=1.58×1017cm−3 and Nd=3.16×1018cm−3, and the junction depth xj=0.05μm. All calculated parameter values are considered as theoretical limit values. In addition, the contribution of BV effect and BPV effect to the output performance of the dual-effect radioisotope battery was investigated. Different scintillator thicknesses lead to different percentages of the two mechanics. In addition, the BV effect and BPV effect output proportion is also affected by the average energy of the radiation source. In the case that the average electron energy on the semiconductor surface is 0.27 MeV, the higher the radioactive source energy, the thicker the scintillator is required, resulting in more BPV effect and less BV effect.

Constructing sulfur-rich interphase to promote the cycle stability of graphite/LiNi0.8Co0.1Mn0.1O2 pouch battery at elevated temperature

Lithium-ion batteries (LIBs) with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes have a high energy density, but their long-cycle performance, especially at high temperature, should still be improved due to the instability of the NCM811 cathode-electrolyte interphase. In this work, 2, 2, 2-Trifluoroethyl p-Toluenesulfonate (TPTS) is introduced as a functional film-forming electrolyte additive design to improve the long-term stability of graphite/NCM811 batteries. The preferential redox reactions of TPTS molecules play a pivotal role in fostering the creation of a sulfur-riched interphase, characterized by low impedance. This interphase works to fortify the interfacial structure, effectively inhibiting the dissolution of transition metal ions. Therefore, in comparison to the graphite/NCM811 pouch batteries lacking additive, TPTS enhance the long-cycle capacity retention from 47 % to 80 % after 450 cycles at 45 °C. What's more, TPTS suppresses outgassing and demonstrates enhanced capacity maintenance for the battery even after storage at 60 °C. This work not only demonstrates the stabilizing impacts of TPTS on the electrode-electrolyte interphase and its enhancement of cycling performance at elevated temperatures but also introduces a novel approach for the practical utilization of functional electrolytes matching high-nickel LIBs.

Achieving Uniform Li Deposition and Suppressed Electrolyte Flammability in Li‐Metal Batteries via Designing Localized High‐Concentration Electrolytes

AbstractThe increasing need for energy storage devices with high energy density has led to significant interest in Li‐metal batteries (LMBs). However, the use of commercial electrolytes in LMBs is problematic due to their flammability, inadequate performance at low temperatures, and tendency to promote the growth of lithium dendrites and other flaws. This study introduces a localized high‐concentration electrolyte (LHCE) that addresses these issues by employing non‐flammable electrolyte components and incorporating carefully designed additives to enhance flame retardancy and low‐temperature performance. By incorporating additives to optimize the electrolyte, it is possible to attain inorganic‐dominated solid electrolyte interphases on both the cathode and anode. This achievement results in a uniform deposition of lithium, as well as the suppression of electrolyte decomposition and cathode deterioration. Consequently, this LHCE achieve over 300 stable cycles for both LiNi0.9Mn0.05Co0.05O2||Li cells and LiCoO2||Li cells, as well as 50 cycles for LiNi0.8Mn0.1Co0.1O2 (NCM811||Li) pouch cells. Furthermore, NCM811||Li cells maintain 84% discharge capacity at −20 °C, in comparison to the capacity at room temperature. The utilization of this electrolyte presents novel perspectives for the safe implementation of LMBs.

Cellulose-based separator woven by double-layer-configuration fibers for high S-load Li-S batteries

Lithium-sulfur (Li-S) battery with high theoretical energy density, has been the most promising next-generation energy storage devices. However, the capacity of the high S-loaded cathode decays rapidly due to the shuttling of soluble polysulfide intermediates between the two electrodes, which seriously inhibits its development. In this work, polyacrylonitrile (PAN) and cellulose composite film (PAN@CE) is designed, which is woven by double-layer configuration fiber. The outer layer of fiber is mainly composed of cellulose, and the inner layer is mainly PAN. From DFT calculations and experiments, the double-layer configuration enriched with nitrogen and oxygen groups can effectively inhibit the shuttle of soluble polysulfides. Meanwhile, the interlaced network structure of PAN@CE improves the electrolyte wettability and provides abundance transport paths for ions. In addition, the film also has good thermal stability. Hence, the cycling stability of Li-S batteries with PAN@CE as separator has been greatly improved. Cellulose-based Li-S battery with 9.1 mg S loading and an E/S ratio of 6.2 μL mg−1 is assembled. Its initial area capacity is 5.67 mAh cm−2. After 200 long cycles, the area capacity keeps above 4.0 mAh cm−2.

Bi‐interlayer Strategy for Modulating NiCoP‐based Heterostructure toward High‐performance Aqueous Energy Storage Devices

AbstractNickel‐cobalt (NiCo) phosphides (NCPs) possess high electrochemical activity, which makes them promising candidates for electrode materials in aqueous energy storage devices, such as supercapacitors and zinc batteries. However, the actual specific capacitance and rate capability of NCPs require further improvement, which can be achieved through reasonable heterostructural design and loading conditions of active materials on substrates. Herein, novel hierarchical Bi‐NCP heterogeneous structures with built‐in electric fields consisting of bismuth (Bi) interlayers (electrodeposited on carbon cloth (CC)) were designed and fabricated to ensure the formation of uniform high‐load layered active materials for efficient charge and ion transport. The resulting CC/Bi‐NCP electrodes showed a uniform, continuous, and high mass loading (>3.5 mg) with a superior capacitance reaching 1200 F⋅g−1 at 1 A⋅g−1 and 4129 mF⋅cm−2 at 1 mA⋅cm−2 combined with high‐rate capability and durable cyclic stability. Moreover, assembled hybrid supercapacitors, supercapatteries, and alkaline zinc batteries constructed using these electrodes delivered high energy densities of 64.4, 81.8, and 319.1 Wh·kg−1, respectively. Overall, the constructed NCPs with excellent aqueous energy storage performance are potential for the development of novel transition metal‐based heterostructure electrodes for advanced energy devices.This article is protected by copyright. All rights reserved

Nanoporous Carbon Materials Derived from Zanthoxylum Bungeanum Peel and Seed for Electrochemical Supercapacitors

In order to prepare biomass-derived carbon materials with high specific capacitance at a low activation temperature (≤700 °C), nanoporous carbon materials were prepared from zanthoxylum bungeanum peels and seeds via the pyrolysis and KOH-activation processes. The results show that the optimal activation temperatures are 700 °C and 600 °C for peels and seeds. Benefiting from the hierarchical pore structure (micropores, mesopores, and macropores), the abundant heteroatoms (N, S, and O) containing functional groups, and plentiful electrochemical active sites, the PAC-700 and SAC-600 derive the large capacities of ~211.0 and ~219.7 F g−1 at 1.0 A g−1 in 6 M KOH within the three-electrode configuration. Furthermore, the symmetrical supercapacitors display a high energy density of 22.9 and 22.4 Wh kg−1 at 7500 W kg−1 assembled with PAC-700 and SAC-600, along with exceptional capacitance retention of 99.1% and 93.4% over 10,000 cycles at 1.0 A g−1. More significantly, the contribution here will stimulate the extensive development of low-temperature activation processes and nanoporous carbon materials for electrochemical energy storage and beyond.

Pressure Tuning and Sn Particle Size Optimization for Enhanced Performance in PbSnF4-Based All-Solid-State Fluoride Ion Batteries.

All-solid-state fluoride ion batteries (ASSFIBs) show remarkable potential as energy storage devices due to their low cost, superior safety, and high energy density. However, the poor ionic conductivity of F- conductor, large volume expansion, and the lack of a suitable anode inhibit their development. In this work, PbSnF4 solid electrolytes in different phases (β- and γ-PbSnF4) are successfully synthesized and characterized. The ASSFIBs composed of β-PbSnF4 electrolytes, a BiF3 cathode, and micrometer/nanometer size (µ-/n-) Sn anodes, exhibit substantial capacities. Compared to the μ-Sn anode, the n-Sn anode with nanostructure exhibits superior battery performance in the BiF3/β-PbSnF4/Sn battery. The optimized battery delivers a high initial discharge capacity of 181.3 mAh g-1 at 8mA g-1 and can be reversibly cycled at 40mA g-1 with a high discharge capacity of over 100.0 mAh g-1 after 120 cycles at room temperature. Additionally, it displays high discharge capacities over 90.0 mAh g-1 with excellent cyclability over 100 cycles under -20°C. Detailed characterization has confirmed that reducing Sn particle size and boosting external pressure are crucial for achieving good defluorination/fluorination behaviors in the Sn anode. These findings pave the way to designing ASSFIBs with high capacities and superior cyclability under different operating temperatures.

Machine-Learning-Assisted Development of Gel Polymer Electrolytes for Protecting Zn Metal Anodes from the Corrosion of Water Molecules.

Rechargeable aqueous zinc-ion batteries (RAZIBs) offer low cost, high energy density, and safety but struggle with anode corrosion and dendrite formation. Gel polymer electrolytes (GPEs) with both high mechanical properties and excellent electrochemical properties are a powerful tool to aid the practical application of RAZIBs. In this work, guided by a machine learning (ML) model constructed based on experimental data, polyacrylamide (PAM) with a highly entangled structure was chosen to prepare GPEs for obtaining high-performance RAZIBs. By controlling the swelling degree of the PAM, the obtained GPEs effectively suppressed the growth of Zn dendrites and alleviated the corrosion of Zn metal caused by water molecules, thus improving the cycling lifespan of the Zn anode. These results indicate that using ML models based on experimental data can effectively help screen battery materials, while highly entangled PAMs are excellent GPEs capable of balancing mechanical and electrochemical properties.

Characteristics and properties of anode materials for lithium-ion batteries

Lithium-ion secondary batteries (LIBs) are battery systems with high energy densities. They are essential components of todays information-rich, mobile societys portable, entertainment, computing, and telecommunications technology. After 1981, most of the research on anode materials mainly focused on the anode containing Li, such as LiAl alloy, LiC alloy, etc. These materials have high prices, unstable cycling performance, and are difficult to be commercialized. The successful commercialization of LIBs began in 1991 with SONYs manufacturing of petroleum coke-based anode materials. Among them, anode plays a crucial role in LIBs. Anode materials that have been commercialized include carbon, alloys, and lithium titanate. Lithium-ion batteries using carbon anode materials and lithium titanate anode materials can meet the needs of electric vehicles (EVs) and large-scale energy storage applications to a certain extent, and alloy anode materials can promote the energy density of LIBs. The properties of the commercialized anode materials are covered in this paper. Next generation anode materials such as silicon anode materials are also introduced.

Inorganic Composition Modulation of Solid Electrolyte Interphase for Fast Charging Lithium Metal Batteries.

The solid electrolyte interphase (SEI) with lithium fluoride (LiF) is critical to the performance of lithium metal batteries (LMBs) due to its high stability and mechanical properties. However, the low Li ion conductivity of LiF impedes the rapid diffusion of Li ions in the SEI, which leads to localized Li ion oversaturation dendritic deposition and hinders the practical applications of LMBs at high-current regions (>3 C). To address this issue, we introduce a fluorophosphated SEI rich with fast ion-diffusing inorganic grain boundaries (LiF/Li3P). By utilizing a sol electrolyte that contains highly dispersed porous LiF nanoparticles modified with phosphorus-containing functional groups, we construct a fluorophosphated SEI and demonstrate the presence of electrochemically-active Li within these fast ion-diffusing grain boundaries (GBs-Li) that are non-nucleated, ensuring the stability of the Li || NCM811 cell for over 1,000 cycles at fast-charging rates of 5 C (11mA cm-2). Additionally, we fabricate a practical, long cycling, and intrinsically safe LMB pouch cell with high energy density (400Wh kg-1). Our work reveals how SEI components and structure design can enable fast-charging LMBs. This article is protected by copyright. All rights reserved.

Recent Progress of Low-Dimensional Metal-Organic Frameworks for Aqueous Zinc-Based Batteries.

Aqueous zinc-based batteries (AZBs) are promising energy storage solutions with remarkable safety, abundant Zn reserve, cost-effectiveness, and relatively high energy density. However, AZBs still face challenges such as anode dendrite formation that reduces cycling stability and limited cathode capacity. Recently, low-dimensional metal-organic frameworks (LD MOFs) and their derivatives have emerged as promising candidates for improving the electrochemical performance of AZBs owing to their unique morphologies, high structure tunability, high surface areas, and high porosity. However, clear guidelines for developing LD MOF-based materials for high-performance AZBs are scarce. In this review, the recent progress of LD MOF-based materials for AZBs is critically examined. The typical synthesis methods and structural design strategies for improving the electrochemical performance of LD MOF-based materials for AZBs are first introduced. The recent noteworthy research achievements are systematically discussed and categorized based on their applications in different AZB components, including cathodes, anodes, separators, and electrolytes. Finally, the limitations are addressed and the future perspectives are outlined for LD MOFs and their derivatives in AZB applications. This review provides clear guidance for designing high-performance LD MOF-based materials for advanced AZBs.

Three Birds with One Stone: Multifunctional Separators Based on SnSe Nanosheets Enable High‐Performance Li‐, Na‐ and K‐Sulfur Batteries

AbstractAlkali metal‐sulfur batteries (MSBs) are one of the most promising next‐generation energy storage technologies due to their high energy density and potential for low cost. They are nonetheless constrained by the sluggish conversion of metal polysulfides (MPS) during the charge/discharge process. Herein, a multifunctional separator able to trap the MPS and catalyze their conversion in the three main MSB chemistries, Li‐, Na‐, and K‐MSBs, is demonstrated. More in detail, SnSe nanosheets are introduced as additive into the cathode side of the glass microfiber (GF) separator of the MSB. Taking lithium‐sulfur batteries (LSBs) as an example, it is demonstrated that the GF‐SnSe separator (GF@SnSe) shows strong chemical affinity to lithium polysulfides (LiPS) and superior catalytic activity, inhibiting the transport of LiPSs to the anode and accelerating their conversion. Combining experimental and calculation results, the SnSe additive is shown to decrease the Li2S decomposition energy barrier. Overall, GF@SnSe separators provide significantly improved LSB rate performance and cycling stability with a 0.049% capacity decay per cycle. Besides, the GF@SnSe separator promotes the electrochemical performance of sodium‐sulfur and potassium‐sulfur batteries. Overall, this work presents a significant advancement in the development of multifunctional separators in LSBs as well as the emerging Na‐S and K‐S systems.

Synergistic effect of interlayered doping and surface modification to improve the performance of Li-rich manganese-based cathode materials

Li-rich manganese-based oxides (LRMOs) with high energy density have been intensively studied, but their practical use as cathode materials for lithium-ion batteries is still impeded by the shortcomings such as low initial coulombic efficiency, voltage decay and poor rate capability. To address these issues, element Nb is selected to bulk dope and simultaneously surface modify the hierarchical Li1.20Mn0.54Co0.13Ni0.13O2 spheres in this work. Synergistic effect of Nb doping and surface modification on the crystalline structure and electrochemical performance of the resultant LRMOs is characterized in detail. The results suggest that Nb5+ ions are doped into the interlayer sites within the crystals while the LiMn2O4 and LiNb3O8 double layers are coated on the primary nanoparticles. The galvanostatic charge-discharge measurements reveal that the optimal LRMO-Nb2 sample can deliver the capacities of 286 and 167 mAh g−1 at the rates of 0.1 C and 5 C, respectively, and retains a capacity of 191 mAh g−1 at 1 C rate after 200 cycles. Ex-situ XRD patterns prove that the layered structure is strongly pillared by the interlayer-doped Nb5+ during the delithiation/lithiation processes. Especially, some lithium vacancies formed around Nb5+ ions can accelerate the diffusion of Li+ ions, which was proved by DFT calculations and experimental results. Our research demonstrates that cooperating of the interlayered doping of Nb5+ with surface coating of LiNb3O8 layer can improve rate capability and cyclability of the resultant LRMOs significantly.