Materials For Rechargeable Batteries Research Articles

Prussian blue analogue derived phosphatized cobalt coupling N-doped carbon system as an efficient oxygen electrocatalyst for rechargeable zinc-air battery

Recently, CoP is considered as a very promising electrode material for rechargeable zinc-air battery (ZAB). In this study, a Prussian blue analogue (Co3[Co(CN)6]2, PBA) derived CoP coupling with N-doped carbon (NC) as an effective oxygen electrocatalyst PBA-CoP/NC was prepared. Notably, as-prepared PBA-CoP/NC has good oxygen reduction reaction (ORR) performance even comparable to Pt/C (0.855 V), with half wave potential reaching 0.847 V. While, it also has satisfactory performance for oxygen evolution reaction (OER). Importantly, the PBA-CoP/NC assembled ZAB exhibits an open circuit potential of 1.62 V, and a peak power density of 119.3 mW cm−2, as well as good stability. This PBA-CoP/NC catalyst would give good reference to developing advanced carbon-based electrocatalyst, also has great potential applied in other energy storage devices.

Alleviated mechanical structure decay and accelerated transport kinetics via KNCHCF@NiHCF core–shell structure for aqueous potassium-ion batteries

The sluggish ion transport and mechanical decay caused by K+ intercalation can hinder the K+ storage ability of Prussian blue analogs (PBAs), potential cathode materials for potassium-ion batteries (PIBs). The construction of composite materials using adjustable chemical components of PB is an effective method to improve cycling stability. In this study, a core–shell structure of KNiCoFe(CN)6@NiFe(CN)6 (KNCHCF@NiHCF) was prepared to utilize the inertness of Ni2+ and the stability of Fe–CN–Ni bonds and enhance the performance of PBAs. Different concentrations of NiHCF coating (Ni-0, Ni-2, Ni-5, and Ni-60) were introduced into the outer layer of KNCHCF using a simple solution precipitation method. The aforementioned core–shell structure and the corresponding built-in electric field enhanced the structural stability and K+/e− transport kinetics of the fabricated materials. And Ni-5 exhibited the best electrochemical performance with excellent durable cycling stability and rate performance. Furthermore, the reversible single-phase insertion and extraction reaction of K+ storage mechanism within the Ni-5 cathode was revealed using ex-/in-situ characterization techniques. This strategy may facilitate the development of other cathode materials for rechargeable metal ion batteries.

Prediction of S-functionalized double-metal TiNbC MXene monolayer as a promising anode material for superior high-capacity mono- and multivalent ion batteries

In search of new electrode materials that improve rechargeable metal-ion batteries’ performance, S-functionalized double-metal TiNbC MXene monolayer (TiNbCS2) is designed, and its properties as an anode material for Li-, Na-, K-, Mg-, Ca-, and Al-ion batteries are investigated employing density functional theory. Due to technical issues during the preparation process, the surface of MXenes is mostly terminated by –O, –OH, and –F functional groups. It is possible to modify the surface by other terminal groups to improve MXenes’ energy storage performance. According to our findings, the TiNbCS2 monolayer, thanks to its metallic behavior, high chemical stability, low diffusion energy barriers, and low open-circuit voltages of these metal cations, is a promising anode material for rechargeable metal-ion batteries. Notably, the adsorption of multilayers of Na+ and Mg2+ cations on the surface of TiNbCS2 provides excellent capacities of 494 mA h g−1 and 988 mA h g−1 for Na- and Mg-ion batteries, respectively. Although the trivalent Al ion may offer a higher energy density, our calculations show that Al3+ ions are not adsorbed onto the surface of the TiNbCS2 monolayer effectively.

Toward Sustainable Polymer Materials for Rechargeable Batteries: Utilizing Natural Feedstocks and Recycling/Upcycling of Polymer Waste.

The ever-increasing demand for rechargeable battery systems in the era of electric vehicles has spurred extensive research into developing polymeric components for batteries, such as separators, polymer electrolytes, and binders. However, current battery systems rely on expensive and nonrenewable resources, which potentially have a negative environmental impact. Therefore, polymer materials derived from natural resources have gained significant attention, primarily due to their cost-effective and environmentally sustainable features. Moreover, natural feedstocks often possess highly polar functional groups and high molecular weights, offering desirable electro-chemo-mechanical features when applied as battery materials. More recently, various recycling and upcycling strategies for polymeric battery components have also been proposed given the substantial waste generation from end-of-life batteries. Recycling polymeric materials includes an overall process of recovering the components from spent batteries followed by regeneration into new materials. Polymer upcycling into battery materials involves transforming daily-used plastic waste into high-value-added battery components. This review aims to give a state-of-the-art overview of contemporary methods to develop sustainable polymeric materials and recycling/upcycling strategies for various battery applications.

Initiating cationic-anionic chemistry with stepwise surface-to-inner conversion in copper selenide superstructures for high-energy rechargeable magnesium batteries

Copper selenides are viewed as the most capable cathode materials for rechargeable magnesium batteries, yet suffer from unsatisfactory energy density due to their low operating voltage plateau (∼0.9 V vs. Mg/Mg2+) and insufficient reversible capacity. Herein, a stepwise conversion from surface cationic-anionic redox to inside electrochemical displacement reaction is realized in copper selenide (Cu2-xSe) superstructure cathodes. A highly reversible high-voltage platform at ∼1.6 V is discovered during discharge process. Ex-situ spectroscopy and microscopy results demonstrate that the high-voltage plateau is contributed by surface Cu2+ charge-carrier transformation and anionic Se2– redox reaction while sufficient inner Cu-Mg replacement conversion at low-voltage region. Following the favorable mechanism, the Cu2-xSe superstructure cathodes can present high specific capacity of 385.4 mAh g–1 at 0.1 A g–1 and outstanding energy density of 426.3 Wh kg–1. Moreover, the Cu2-xSe superstructure cathodes also maintain a reversible capacity of 223.6 mAh g–1 over 700 cycles with 0.0147 % capacity degradation per cycle at 1.0 A g–1 and long-term charge-discharge lifetime for 3000 cycles at 5.0 A g–1. This research reports a new Mg2+ storage mechanism for copper selenide cathodes and provides novel route to develop high-energy-density rechargeable magnesium batteries.

First-principles study on the electrochemical properties of Na-ion-intercalatable heterostructures formed by transitional metal dichalcogenides and blue phosphorus

Extensive first-principles calculations have been performed to examine the electrochemical properties of Na-ion-intercalatable heterostructures formed by transitional metal dichalcogenides (MS2, where M = Ti, V, Nb and Mo) and blue phosphorus (BlueP), which have been reported as potential anode materials for rechargeable sodium-ion batteries. Upon formation of heterostructures, much improved structural stabilities have observed compared with the pristine MS2 and BlueP. Metallic T-TiS2, T-MoS2, H(T)-VS2 and H(T)-NbS2 would retain the conductive character after formation of heterostructures with BlueP, however, H-TiS2/BlueP and H-MoS2/BlueP would undergo a semiconductor to metallic transition accompanied by Na intercalation. Moreover, the presence of relatively low diffusion barriers ranging from 0.04 eV to 0.08 eV, coupled with the suitable average open-circuit voltage spanning from 0.12 eV to 0.89 eV, guarantee exceptional charge-discharge rates and ensure the safety of battery performance. Among these heterostructures, H(T)-NbS2/BlueP and T-TiS2/BlueP exhibit best Na adsorption ability of up to 4 layers, corresponding to theoretical capacities of 570.2 and 746.7 mAh/g, respectively. These encouraging properties indicate that T-TiS2/BlueP and H(T)-NbS2/BlueP could serve as suitable anode materials for high-performance sodium-ion batteries.

Interfacial modulation of bifunctional electrolyte additive engineering for dendrite-free and robust lithium metal anode

Anode materials for rechargeable electric car batteries are obtained from Li-metal owing to their extremely high specific capacity and low redox potential. Unfortunately, safety concerns related to dendrite formation on the anode surface caused by the uneven distribution of Li-ions during the discharge process interfere with the use of Li-metal in industrial batteries. In this study, methyl vinyl sulfone (MVS), a sulfone-based functional electrolyte additive, is used in an additive engineering strategy to control Li-electrolyte interactions and address the aforementioned problems. Li dendrite growth may be restricted, and transition metal degradation on the surface of the cathode can be reduced by the MVS-derived functional electrolyte additive interfacial layer. The electrochemical performance of an ethylene carbonate/dimethyl carbonate (EC/DMC) + 1 wt% MVS Li-metal anode of a Li||Li symmetric cell exhibits remarkable cycle stability, maintaining a low overvoltage for over 750 h at 1 mA cm−2, and capacity of 1 mA h cm−2. Additionally, LiNi0.8Co0.1Mn0.1O2 (NCM811) full cells with the MVS additive exhibit enhanced electrochemical stability for 250 cycles at a current density of 100 mA g−1. This study provides an innovative approach for stabilizing the metal-electrolyte interfacial layer that may be used for practical applications in metal-based rechargeable batteries.

Constructing Cu9S5@CuSe heterostructures under microwave irradiation for rechargeable magnesium batteries

Copper chalcogenides are believed as the prospective cathode materials for rechargeable magnesium batteries. However, their practical application is seriously restricted by slow diffusion and reaction kinetics due to the large charge/radius ratio of divalent Mg2+ ions. Herein, a simple two-step microwave-assisted synthesis method is rationally developed to construct Cu9S5@CuSe heterostructures as the capable cathode materials for rechargeable magnesium batteries. Two-dimensional CuSe nanosheets are vertically grown on the surface of single-crystal Cu9S5 substrate through selenation reaction under microwave irradiation to form the mixed-dimensional heterostructures. Electrochemical measurements reveal that the as-synthesized Cu9S5@CuSe heterostructures show high reversible capacity of 240 mAh g−1 and good long-term cyclic stability with approximate 0.013 % capacity decay per cycle at 500 mA g−1 within 1000 cycles. Furthermore, the obviously enhanced rate capability can be achieved in comparison with that of single-crystal Cu9S5 substrate and CuSe nanoparticles. Ex-situ X-ray photoelectron spectroscopy and X-ray diffraction characterizations reveal favourable electrochemical conversion reaction over the Cu9S5@CuSe heterostructure cathode. The superior electrochemical properties are attributed to the optimized diffusion kinetics within the unique heterostructure. This research offers a valuable strategy to develop high-performance cathode materials with favourable kinetics for magnesium batteries.

Coal-based carbon nanosheets contained carbon microfibers modified with grown carbon nanotubes as efficient air electrode material for rechargeable zinc-air batteries

Coal-based oxygen electrocatalysts hold immense promise for cost-effective applications in rechargeable Zn-air batteries (ZABs) and the value-added, clean utilization of traditional coal resources. Herein, an electrospun membrane electrode comprising coal-derived carbon nanosheets and directly grown carbon nanotubes (CNS/CMF@CNT) was successfully synthesized. The hierarchical porous structure of the electrode, composed of multiple components, significantly facilitates mass and ion transportation, resulting in exceptional electrochemical performance. Employing Fe as the catalyst for CNT growth, the CNS/CMF@CNT electrode exhibits a remarkable onset potential of 0.96 V and a half-wave potential of 0.87 V in the oxygen reduction reaction (ORR). In-situ surface-enhanced Raman spectroscopy reveals that hydroxyl radical desorption on the surface of CNS/CMF@CNT(Fe) is the rate-determining step of the ORR. Notably, the aqueous ZAB featuring the CNS/CMF@CNT(Fe) electrode achieved a peak power density of 216.0 mW cm−2 at a current density of 414 mA cm−2 and maintained a voltage efficiency of 65.1 % after 2000 charge/discharge cycles at 5 mA cm−2. Furthermore, the all-solid-state ZAB incorporating this electrode displayed an open-circuit voltage of 1.43 V, a peak power density of 70.1 mW cm−2 at a current density of 110 mA cm−2, and a voltage efficiency of 66.5 % after 150 charge/discharge cycles. The utilization of abundant coal as the raw material for electrode fabrication not only brings conceivable economic benefits in ZAB construction, but also commendably advances the effective application of traditional coal resources in a more sustainable manner.

Interfacial bonding enhances MXene/Sb2Se3 composites toward cyclic stability and fast aluminum storage

Metal-chalcogenides have been extensively studied as electrode materials for rechargeable ion batteries due to their high theoretical specific capacity and high abundance. Although promising, these materials face challenges related to slow electrochemical kinetics, pronounced structural distortions, and severe shuttle effects. These issues have seriously hindered the practical application of metal-chalcogenides in ion batteries. This work presents a novel approach to form interfacial binding bonds and in situ generation of antimony selenide (Sb2Se3) on MXene by electrostatic adsorption. This innovative strategy enhances the reversible capacity and cycling stability of Sb2Se3 and effectively improves the electrochemical kinetics and shuttle effect. Ex-situ characterization elucidates the distinctive energy storage mechanism of the Ti3C2/Sb2Se3 cathode and the inhibitory effect of MXene on the dissolution of reaction intermediates into the electrolyte. Additionally, the improvement in charge transfer and ion diffusion due to the introduction of MXene was validated through density functional theory calculations. This work offers new insights into enhancing the stability of metal-chalcogenides and understanding the energy storage mechanism of antimony-based selenides in ion batteries.

Influence of iron phosphate on the performance of lithium iron phosphate as cathodic materials in rechargeable lithium batteries

Influence of iron phosphate on the performance of lithium iron phosphate as cathodic materials in rechargeable lithium batteries

Rational Regulation of High-Voltage Stability in Potassium Layered Oxide Cathodes.

Layered oxide cathode materials may undergo irreversible oxygen loss and severe phase transitions during high voltage cycling and may be susceptible to transition metal dissolution, adversely affecting their electrochemical performance. Here, to address these challenges, we propose synergistic doping of nonmetallic elements and in situ electrochemical diffusion as potential solution strategies. Among them, the distribution of the nonmetallic element fluorine within the material can be regulated by doping boron, thereby suppressing manganese dissolution through surface enrichment of fluorine. Furthermore, in situ electrochemical diffusion of fluorine from the surface into the bulk of the materials after charging reduces the energy barrier of potassium ion diffusion while effectively inhibiting irreversible oxygen loss under high voltage. The modified K0.5Mn0.83Mg0.1Ti0.05B0.02F0.1O1.9 layered oxide cathode exhibits a high capacity of 147 mAh g-1 at 50 mA g-1 and a long cycle life of 2200 cycles at 500 mA g-1. This work demonstrates the efficacy of synergistic doping and in situ electrochemical diffusion of nonmetallic elements and provides valuable insights for optimizing rechargeable battery materials.

Organic Electrode Materials for Energy Storage and Conversion: Mechanism, Characteristics, and Applications.

ConspectusLithium ion batteries (LIBs) with inorganic intercalation compounds as electrode active materials have become an indispensable part of human life. However, the rapid increase in their annual production raises concerns about limited mineral reserves and related environmental issues. Therefore, organic electrode materials (OEMs) for rechargeable batteries have once again come into the focus of researchers because of their design flexibility, sustainability, and environmental compatibility. Compared with conventional inorganic cathode materials for Li ion batteries, OEMs possess some unique characteristics including flexible molecular structure, weak intermolecular interaction, being highly soluble in electrolytes, and moderate electrochemical potentials. These unique characteristics make OEMs suitable for applications in multivalent ion batteries, low-temperature batteries, redox flow batteries, and decoupled water electrolysis. Specifically, the flexible molecular structure and weak intermolecular interaction of OEMs make multivalent ions easily accessible to the redox sites of OEMs and facilitate the desolvation process on the redox site, thus improving the low-temperature performance, while the highly soluble nature enables OEMs as redox couples for aqueous redox flow batteries. Finally, the moderate electrochemical potential and reversible proton storage and release of OEMs make them suitable as redox mediators for water electrolysis. Over the past ten years, although various new OEMs have been developed for Li-organic batteries, Na-organic batteries, Zn-organic batteries, and other battery systems, batteries with OEMs still face many challenges, such as poor cycle stability, inferior energy density, and limited rate capability. Therefore, previous reviews of OEMs mainly focused on organic molecular design for organic batteries or strategies to improve the electrochemical performance of OEMs. A comprehensive review to explore the characteristics of OEMs and establish the correlation between these characteristics and their specific application in energy storage and conversion is still lacking.In this Account, we initially provide an overview of the sustainability and environmental friendliness of OEMs for energy storage and conversion. Subsequently, we summarize the charge storage mechanisms of the different types of OEMs. Thereafter, we explore the characteristics of OEMs in comparison with conventional inorganic intercalation compounds including their structural flexibility, high solubility in the electrolyte, and appropriate electrochemical potential in order to establish the correlations between their characteristics and potential applications. Unlike previous reviews that mainly introduce the electrochemical performance progress of different organic batteries, this Account specifically focuses on some exceptional applications of OEMs corresponding to the characteristics of organic electrode materials in energy storage and conversion, as previously published by our groups. These applications include monovalent ion batteries, multivalent ion batteries, low-temperature batteries, redox flow batteries with soluble OEMs, and decoupled water electrolysis employing organic electrodes as redox mediators. We hope that this Account will make an invaluable contribution to the development of organic electrode materials for next-generation batteries and help to unlock a world of potential energy storage applications.

Improved rate and cycling capability of V2O5@MoS2 nanocomposites as an advanced cathode material for rechargeable aqueous zinc-ion batteries

Owing to the benefits of higher energy density, reliable safety, and eco-friendliness, rechargeable aqueous zinc (Zn)-ion batteries (RAZIBs) are employed in energy storage applications. Nevertheless, the enhancement of potential cathodes is hindered by low reversibility and sluggish Zn-ion diffusion kinetics, causing deficient rate capability and modest cycling performance. Vanadic anhydride (V2O5) provides a potential in RAZIBs from its layered structure and superior capacity. Herein, molybdenum disulfide (MoS2) was combined into the V2O5 to form V2O5@MoS2 nanocomposites (NCs) via a simple hydrothermal method. The V2O5@MoS2 NCs enable Zn ions to migrate effectively between layers and stabilize volume changes during the insertion/extraction process. Moreover, the presence of MoS2 as a mediator in the framework produces additional defects, which leads to an enhanced storage area for Zn ions. The optimized V2O5@MoS2–2 NCs exhibited a cycling capacity of 230.74 mA h g−1 at 0.5 A g−1, superior rate performance (73.59 mA h g−1 at 30 A g−1), and excellent long-term cycling stability (108.16 mA h g−1 at 10 A g−1 over 6000 cycles), surpassing those of V2O5@MoS2–1, V2O5@MoS2–3, V2O5, and MoS2 counterparts. Such fascinating properties reveal that the proposed composite materials as a progressive cathode for RAZIBs.

Bimetallic Selenide CuFeSe2 as Mg‐Storage Material for Rechargeable Magnesium Batteries

AbstractRechargeable magnesium batteries (RMBs) are appealing alternatives for energy storage systems based on the high theoretical capacity, low price and high security of the Mg metal anode. Nevertheless, the shortage of high‐performance cathode materials severely obstructs its development. As an important conversion material, transition metal selenides, with desirable theoretical capacity and weak bond energy (Mg−Se), have attracted more attention in recent years. In this study, CuFeSe2 (CFS) nanoparticles were produced by a hydrothermal approach and its feasibility as a cathode material for RMBs was further investigated. Given the synergistic effect between Cu and Fe, the optimized CFS shows a reversible capacity of 120 mAh g−1 at 100 mA g−1, outstanding long‐term cyclability (86 mAh g−1 at 1 A g−1 after 600 cycles), and prominent rate capability (85 mAh g−1 at 1 A g−1). Density functional theory (DFT) computations conclude CFS exhibits a suitable migration barrier for Mg2+ along the tunnel of 0.92 eV. An in‐depth investigation of the mechanism demonstrates that the Mg storage process can be divided into solid solution reaction and the conversion processes by ex‐situ techniques. This work contributes to further investigate the Mg2+ storage mechanism of cathode materials for RMBs.

Heavily vanadium-doped LiFePO4 olivine as electrode material for Li-ion aqueous rechargeable batteries

Since LiFePO4 batteries play a major role in the transition to safe, more affordable and sustainable energy production, numerous strategies have been applied to modify LFP cathode, with the aim of improving its electrochemistry. In this contribution, a highly vanadium-doped LiFe0.9V0.1PO4/C composite (LFP/C-10V) is synthesized using the glycine combustion method and characterized by x-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Thermogravimetry Differential Thermal Analysis (TGDTA) and Cyclic Voltammetry (CV). It is shown that 10wt.% of vanadium can substitute Fe positions, thus decreasing unit cell volume, which is followed by generation of Li3V2PO4 traces, as detected by CV. High vanadium doping does not change the carbon content in the composite (≈13 wt%) but improves its electronic conductivity and electrochemical performance in both aqueous and organic electrolytes. The reversibility and current response are increasing following the trend: LFP/C, LFP/C -3mol%V, LFP/C - 5 mol % and LFP/C-10 mol %. The best specific capacity is obtained for the most highly doped olivine, which exhibits a reversible process at 1 mV s−1 in an aqueous electrolyte, thus showing a peak-to-peak distance of 56 mV. The high capacity of LFPC-10V is measured in both LiNO3 and NaNO3 electrolytes amounting to around 100 mAh g−1 at 20 mV s−1. Still, the material is only stable in LiNO3 electrolyte, making it more suitable for Li than Na-ion aqueous rechargeable batteries.

Achieving Highly Stable Zn Metal Anodes at Low Temperature via Regulating Electrolyte Solvation Structure.

Zinc metal is an attractive anode material for rechargeable aqueous Zn-ion batteries (ZIBs). However, the dendrite growth, water-induced parasitic reactions, and freezing problem of aqueous electrolyte at low temperatures are the major roadblocks that hinder the widely commercialization of ZIBs. Herein, tetrahydrofuran (THF) is proposed as the electrolyte additive to improve the reversibility and stability of Zn anode. Theoretical calculation and experimental results reveal that the introduction of THF into the aqueous electrolyte can optimize the solvation structure which can effectively alleviate the H2O-induced side reactions and protect the Zn anode from corrosion. Moreover, THF can act as a hydrogen bond acceptor to interact with H2O, which can greatly reduce the activity of free H2O in electrolytes and improve the low-temperature electrochemical performance of Zn anode. As a result, the Zn anodes demonstrate high cyclic stability for 2800h at 27°C and over 4000h at -10°C at 1.0mA cm-2 /1.0mAhcm-2. The full cell exhibits excellent cyclic stability and rate capability at 27 and -10°C. This work is expected to provide a new approach to regulate the aqueous electrolyte and Zn anode interface chemistry for highly stable and reversible Zn anodes.

High mass loading potassium ion stabilized manganese dioxide nanowire forests for rechargeable Zn batteries

Manganese dioxide (MnO2) represents an ideal cathode material for rechargeable aqueous Zn batteries due to its high theoretical capacity (308 mAh g−1), suitable potential (1.4 V vs. Zn2+/Zn), natural abundance, and negligible toxicity. However, the capacity and rate capability of MnO2 deteriorate significantly in thick electrodes owing to its low electrical and ionic conductivities. Herein, we report the design of high mass loading potassium ion stabilized α-MnO2 (K0.133MnO2) nanowire forests on carbon cloth through a seed-assisted hydrothermal method for Zn batteries. The vertically aligned K0.133MnO2 nanowire forests with uninterrupted charge transport afford a high area capacity of 3.54 mAh cm−2 and a capacity retention of 79.2% over 1000 cycles in aqueous electrolyte. Moreover, the high area capacity and cyclability can be readily transferred to quasi-solid-state devices.

Lithiophilic ZnCu alloy sites on copper current collector for high performance Li metal anode

Lithium (Li) metal has been widely regarded as the optimal anode material for the high-energy density rechargeable batteries, due to its ultrahigh theoretical specific capacity and lowest electrochemical potential. However, the formation of Li dendrites presents a significant safety concern, which limits its practical application. In this paper, to address this issue, an efficient and cost-effective strategy was proposed to prepare a zinc-copper composite collector (ZCC) with outstanding electrochemical performance, which can effectively suppress the formation of lithium dendrites. The lithophilic surface with ZnCu alloy nanoparticles was achieved through physical vapor deposition followed by annealing treatment. The ZCC collector enables dendrite-free deposition of Li due to its negligible nucleation overpotential. Even at high area capacity of 3 mAh cm−2 at 1 mA cm−2 in half-cells, the ZCC exhibits exceptional cycling performance and high coulomb efficiency. Preloaded with Li, the composite electrode (Li/ZCC) delivers an enhanced lifespan with low overpotential evidently. Matched with LiFePO4 (LFP) cathode, LFP||Li/ZCC full cells reveal a superior cycling stability with enhanced capacity retention of 85 % (after 1000 cycles at 1 C) and 87 % (after 800 cycles at 3 C) respectively.

A Fast-Charge Graphite Anode with a Li-Ion-Conductive, Electron/Solvent-Repelling Interface.

Graphite has been serving as the key anode material of rechargeable Li-ion batteries, yet is difficultly charged within a quarter hour while maintaining stable electrochemistry. In addition to a defective edge structure that prevents fast Li-ion entry, the high-rate performance of graphite could be hampered by co-intercalation and parasitic reduction of solvent molecules at anode/electrolyte interface. Conventional surface modification by pitch-derived carbon barely isolates the solvent and electrons, and usually lead to inadequate rate capability to meet practical fast-charge requirements. Here we show that, by applying a MoOx-MoNx layer onto graphite surface, the interface allows fast Li-ion diffusion yet blocks solvent access and electron leakage. By regulating interfacial mass and charge transfer, the modified graphite anode delivers a reversible capacity of 340.3 mAh g-1 after 4000 cycles at 6 C, showing promises in building 10-min-rechargeable batteries with a long operation life.