Fast-Charging, Binder-Free Lithium Battery Cathodes Enabled via Multidimensional Conductive Networks.

To meet the growing demands in both energy and power densities of lithium ion batteries, electrode structures must be capable of facile electron and ion transport while minimizing the content of electrochemically inactive components. Herein, binder-free LiFePO4 (LFP) cathodes are fabricated with a multidimensional conductive architecture that allows for fast-charging capability, reaching a specific capacity of 94 mAh g-1 at 4 C. Such multidimensional networks consist of active material particles wrapped by 1D single-walled carbon nanotubes (CNTs) and bound together using 2D MXene (Ti3C2Tx) nanosheets. The CNTs form a porous coating layer and improve local electron transport across the LFP surface, while the Ti3C2Tx nanosheets provide simultaneously high electrode integrity and conductive pathways through the bulk of the electrode. This work highlights the ability of multidimensional conductive fillers to realize simultaneously superior electrochemical and mechanical properties, providing useful insights into future fast-charging electrode designs for scalable electrochemical systems.

Balancing the Ion/Electron Transport of Graphite Anodes by a La-Doped TiNb2O7 Functional Coating for Fast-Charging Li-Ion Batteries.

A functional coating layer (FCL) is widely applied in fast-charging lithium-ion batteries to improve the sluggish Li+ transport kinetics of traditional graphite anodes. However, blindly increasing the Li+ conductivity for FCL reduces the overall electron conductivity of the anodes. Herein, we decoupled the effect of La-doping on TiNb2O7 (TNO) in terms of the phase evolution, Li+/electron transport, and lithiation behavior, and then proposed a promising La0.1TNO FCL with balanced Li+/electron transport for a fast-charging graphite anode. By optimizing the doping concentration of La, more holes are introduced into the TNO as electron carriers without causing lattice distortion, thus maintaining the fast Li+ diffusion channel in TNO. As a result, the graphite with La0.1TNO FCL delivers an excellent capacity of 220.2 mAh g-1 (96.3% retention) after 450 cycles at 3 C, nearly twice that of the unmodified one.

New Emerging Fast Charging Microscale Electrode Materials.

Fast charging lithium (Li)-ion batteries are intensively pursued for next-generation energy storage devices, whose electrochemical performance is largely determined by their constituent electrode materials. While nanosizing of electrode materials enhances high-rate capability in academic research, it presents practical limitations like volumetric packing density and high synthetic cost. As an alternative to nanosizing, microscale electrode materials cannot only effectively overcome the limitations of the nanosizing strategy but also satisfy the requirement of fast-charging batteries. Therefore, this review summarizes the new emerging microscale electrode materials for fast charging from the commercialization perspective. First, the fundamental theory of electronic/ionic motion in both individual active particles and the whole electrode is proposed. Then, based on these theories, the corresponding optimization strategies are summarized toward fast-charging microscale electrode materials. In addition, advanced functional design to tackle the mechanical degradation problems related to next generation high capacity alloy- and conversion-type electrode materials (Li, S, Si et al.) for achieving fast charging and stable cycling batteries. Finally, general conclusions and the future perspective on the potential research directions of microscale electrode materials are proposed. It is anticipated that this review will provide the basic guidelines for both fundamental research and practical applications of fast-charging batteries.

3D Pathways Enabling Highly-Efficient Lithium Reservoir for Fast-Charging Batteries.

Enhancing the mobility of lithium-ions (Li+) through surface engineering is one of major challenges facing fast-charging lithium-ion batteries (LIBs). In case of demanding charging conditions, the use of a conventional artificial graphite (AG) anode leads to an increase in operating temperature and the formation of lithium dendrites on the anode surface. In this study, a biphasic zeolitic imidazolate framework (ZIF)-AG anode, designed strategically and coated with a mesoporous material, is verified to improve the pathways of Li+ and electrons under a high charging current density. In particular, the graphite surface is treated with a coating of a ZIF-8-derived carbon nanoparticles, which addresses sufficient surface porosity, enabling this material to serve as an electrolyte reservoir and facilitate Li+ intercalation. Moreover, the augmentation in specific surface area proves advantageous in reducing the overpotential for interfacial charge transfer reactions. In practical terms, employing a full-cell with the biphasic ZIF-AG anode results in a shorter charging time and improved cycling performance, demonstrating no evidence of Li plating during 300 cycles under 3.0 C-charging and 1.0 C-discharging. The research endeavors to contribute to the progress of anode materials by enhancing their charging capability, aligning with the increasing requirements of the electric vehicle applications.

In Situ Formation of Heterojunction in Composite Lithium Anode Facilitates Fast and Uniform Interfacial Ion Transport.

Lithium metal is a highly promising anode for next-generation high-energy-density rechargeable batteries. Nevertheless, its practical application faces challenges due to the uncontrolled lithium dendrites growth and infinite volumetric expansion during repetitive cycling. Herein, a composite lithium anode is designed by mechanically rolling and pressing a cerium oxide-coated carbon textile with lithium foil (Li@CeO2/CT). The in situ generated cerium dioxide (CeO2) and cerium trioxide (Ce2O3) form a heterojunction with a reduced lithium-ion migration barrier, facilitating the rapid lithium ions migration. Additionally, both CeO2 and Ce2O3 exhibit higher adsorbed energy with lithium, enabling faster and more distributed interfacial transport of lithium ions. Furthermore, the high specific surface area of 3D skeleton can effectively reduce local current density, and alleviate the lithium volumetric changes upon plating/stripping. Benefiting from this unique structure, the highly compact and uniform lithium deposition is constructed, allowing the Li@CeO2/CT symmetric cells to maintain a stable cycling for over 500 cycles at an exceptional high current density of 100 mA cm-2. When paired with LiNi0.91Co0.06Mn0.03O2 (NCM91) cathode, the cell achieves 74.3% capacity retention after 800 cycles at 1 C, and a remarkable capacity retention of 81.1% after 500 cycles even at a high rate of 4  C.

Heterogeneous MoS2 Nanosheets on Porous TiO2 Nanofibers toward Fast and Reversible Sodium-Ion Storage.

2D layered molybdenum disulfide (MoS2) has garnered considerable attention as an attractive electrode material in sodium-ion batteries (SIBs), but sluggish mass transfer kinetic and capacity fading make it suffer from inferior cycle capability. Herein, hierarchical MoS2 nanosheets decorated porous TiO2 nanofibers (MoS2 NSs@TiO2 NFs) with rich oxygen vacancies are engineered by microemulsion electrospinning method and subsequent hydrothermal/heat treatment. The MoS2 NSs@TiO2 NFs improves ion/electron transport kinetic and long-term cycling performance through distinctive porous structure and heterogeneous component. Consequently, the electrode exhibits excellent long-term Na storage capacity (298.4 mAh g-1 at 5 A g-1 over 1100 cycles and 235.6 mAh g-1 at 10 A g-1 over 7200 cycles). Employing Na3V2(PO4)3 as cathode, the full cell maintains a desirable capacity of 269.6 mAh g-1 over 700 cycles at 1.0 A g-1. The stepwise intercalation-conversion and insertion/extraction endows outstanding Na+ storage performance, which yields valuable insight into the advancement of fast-charging and long-cycle life SIBs anode materials.

Design and Realization of Visual and Contact-Type Fast Charging Power Source.

Charging power supplies with both fast and visualization functions have a wide range of applications in the information and new energy industries. In this paper, the visualized and contact-type fast charging power supply based on WO3 film and Zn sheet is presented, and the prototype devices are fabricated. Different with the charging method of conventional batteries, charging is achieved by a Zn sheet contacting with a WO3 film moistened with water, resulting in a rapid discoloration of WO3. Theoretical investigation indicates that the interaction between Zn sheet and water molecules is the primary cause of the color change in the WO3 film. The WO3 film completes the colouring state within 10 s in the presence of Zn sheet and water, and the open-circuit voltage of the device is 0.7 V, which can be used to drive various electronics by series-parallel connection. This research introduces a novel method to induce colouring of WO3 films and proposes a fast charging mode different from traditional power sources. It provides valuable insights for the future development of fast charging in the field of electrical energy.

10†µm-Level TiNb2 O7 Secondary Particles for Fast-Charging Lithium-Ion Batteries.

TiNb2 O7 with Wadsley-Roth phase delivers double theoretical specific capacity and similar working potential in comparison to spinel Li4 Ti5 O12 , the commercial high-rate anode material, and thus can enable much higher energy density of lithium-ion batteries. However, the inter-particle resistance within the high-mass-loading TiNb2 O7 electrode would impede the capacity release for practical application, especially under fast-charging conditions. Herein, 10-20 µm-size carbon-coated TiNb2 O7 secondary particle (SP-TiNb2 O7 ) consisting of initial micro-scale TiNb2 O7 particles (MP-TiNb2 O7 ) was fabricated. The high crystallinity of active material could enable fast-charge diffusion and electrochemical reaction rate within particles, and the small number of stacking layers of SP-TiNb2 O7 could reduce the large inter-particle resistance that regular particle electrode often possess and achieve high compaction density of electrodes with high mass loading. The investigation on materials structure and electrochemical reaction kinetics verified the advances of the as-fabricated SP-TiNb2 O7 in achieving superior electrochemical performance. The SP-TiNb2 O7 exhibited high reversible capacity of 292.7 mAh g-1 in the potential range of 1-3 V (Li+ /Li) at 0.1 C, delivering high-capacity release of 94.3 %, and high capacity retention of 86 % at 0.5 C for 250 cycles in half cell configuration. Particularly, the advances of such an anode were verified in practical 5 Ah-level laminated full pouch cell. The as-assembled LiFePO4 ||TiNb2 O7 full cell exhibited a high capacity of 5.08 Ah at high charging rate of 6 C (77.9 % of that at 0.2 C of 6.52 Ah), as well as an ultralow capacity decay rate of 0.0352 % for 250 cycles at 1 C, suggesting the great potential for practical fast-charging lithium-ion batteries.

Amorphous Anode Materials for Fast-charging Lithium-ion Batteries.

Fast-charging technology is set to revolutionize the field of lithium-ion batteries (LIBs), driving the creation of next-generation devices with the ability to get charged within a short span of time. From the anode perspective, it is of paramount importance to design materials that can withstand continuous Li+ insertion/deinsertion at high charging rates and still remain unaffected by factors such as mechanical fractures, electrolyte side reactions, polarisation, lithium plating and heat generation. Herein, the recent advancements in the design of amorphous materials as anodes for fast-charging LIBs have been discussed. While the development of this particular class of materials for application in high-rate anodes has been paid limited attention in recent literature, it holds immense promise for improving the fast-charging capabilities. This concept summarizes the recent strides made in this emerging field, outlining the strategies employed in the design of amorphous anodes and emphasizing the crucial role played by the amorphous nature in achieving fast-charging performance. Further, the successive initiatives that can be undertaken to drive the progress of amorphous materials for fast charging LIBs have also been detailed, which could potentially improve their commercial viability.

Scalable Fast-Charging Aligned Battery Electrodes Enabled by Bidirectional Freeze-Casting.

Over the past few years, lithium-ion batteries have been extensively adopted in electric transportation. Meanwhile, the energy density of lithium-ion battery packs has been significantly improved, thanks to the development of materials science and packing technology. Despite recent progress in electric vehicle cruise ranges, the increase in battery charging rates remains a pivotal problem in electrodes with commercial-level mass loadings. Herein, we develop a scalable strategy that incorporates bidirectional freeze-casting into the conventional tape-casting method to fabricate energy-dense, fast-charging battery electrodes with aligned structures. The vertically lamellar architectures in bidirectional freeze-cast electrodes can be roll-to-roll calendered, forming the tilted yet aligned channels. These channels enable directional pathways for efficient lithium-ion transport in electrolyte-filled pores and thus realize fast-charging capabilities. In this work, we not only provide a simple yet controllable approach for building the aligned electrode architectures for fast charging but also highlight the significance of scalability in electrode fabrication considerations.

Unlocking Liquid Sulfur Chemistry for Fast-Charging Lithium-Sulfur Batteries.

A recent study of liquid sulfur produced in an electrochemical cell has prompted further investigation into regulating Li-S oxidation chemistry. In this research, we examined the liquid-to-solid sulfur transition dynamics by visually observing the electrochemical generation of sulfur on a graphene-based substrate. We investigated the charging of polysulfides at various current densities and discovered a quantitative correlation between the size and number density of liquid sulfur droplets and the applied current. However, the areal capacities exhibited less sensitivity. This observation offers valuable insights for designing fast-charging sulfur cathodes. By incorporating liquid sulfur into Li-S batteries with a high sulfur loading of 4.2 mg cm-2, the capacity retention can reach ∼100%, even when increasing the rate from 0.1 to 3 C. This study contributes to a better understanding of the kinetics involved in the liquid-solid sulfur growth in Li-S chemistry and presents viable strategies for optimizing fast-charging operations.

Materials recovery from NMC batteries with water as the sole solvent.

We report an environmentally benign recycling approach for large-capacity nickel manganese cobalt (NMC) batteries through the electrochemical concentration of lithium on the anode and subsequent recovery with only water. Cycling of the NMC pouch cells indicated the potential for maximum lithium recovery at a 5C charging rate. The anodes extracted from discharged and disassembled cells were submerged in deionized water, resulting in lithium dissolution and graphite recovery from the copper foils. A maximum of 13 mg of lithium salts per 100 mg of the anode, copper current collector, and separator was obtained from NMC pouch cell cycled at a 4C charging rate. The lithium salts extracted from batteries cycled at low C-rates were richer in lithium carbonate, while the salts from batteries cycled at high C-rates were richer in lithium oxides and peroxides, as determined by X-Ray photoelectron spectroscopy. The present method can be successfully used to recover all the pouch cell components: lithium, graphite, copper, and aluminum current collectors, separator, and the cathode active material.

Li3PO4-Enriched SEI on Graphite Anode Boosts Li+ De-Solvation Enabling Fast-Charging and Low-Temperature Lithium-Ion Batteries.

Li+ de-solvation at solid-electrolyte interphase (SEI)-electrolyte interface stands as a pivotal step that imposes limitations on the fast-charging capability and low-temperature performance of lithium-ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li+ de-solvation and deciphering their mechanisms, as a design principle for the interfacial structure of anode materials, is still a challenge. Herein, we conducted a systematic exploration of the influence exerted by various inorganic components (Li2CO3, LiF, Li3PO4) found in the SEI on their role in promoting the Li+ de-solvation. The findings highlight that Li3PO4-enriched SEI effectively reduces the de-solvation energy due to its ability to attenuate the Li+-solvent interaction, thereby expediting the de-solvation process. Building on this, we engineer Li3PO4 interphase on graphite (LPO-Gr) anode via a simple solid-phase coating, facilitating the Li+ de-solvation and building an inorganic-rich SEI, resulting in accelerated Li+ transport crossing the electrode interfaces and interphases. Full cells using the LPO-Gr anode can replenish its 80 % capacity in 6.5 minutes, while still retaining 70 % of the room temperature capacity even at -20 °C. Our strategy establishes connection between the de-solvation characteristics of the SEI components and the interfacial structure design of anode materials for high performance LIBs.

Rational Lithium Salt Molecule Tuning for Fast Charging/Discharging Lithium Metal Battery.

The electrolytes for lithium metal batteries (LMBs) are plagued by a low Li+ transference number (T+) of conventional lithium salts and inability to form a stable solid electrolyte interphase (SEI). Here, we synthesized a self-folded lithium salt, lithium 2-[2-(2-methoxy ethoxy)ethoxy]ethanesulfonyl(trifluoromethanesulfonyl) imide (LiETFSI), and comparatively studied with its structure analogue, lithium 1,1,1-trifluoro-N-[2-[2-(2-methoxyethoxy)ethoxy)]ethyl]methanesulfonamide (LiFEA). The special anion chemistry imparts the following new characteristics: i) In both LiFEA and LiETFSI, the ethylene oxide moiety efficiently captures Li+, resulting in a self-folded structure and high T+ around 0.8. ii) For LiFEA, a Li-N bond (2.069 Å) is revealed by single crystal X-ray diffraction, indicating that the FEA anion possesses a high donor number (DN) and thus an intensive interphase "self-cleaning" function for an ultra-thin and compact SEI. iii) Starting from LiFEA, an electron-withdrawing sulfone group is introduced near the N atom. The distance of Li-N is tuned from 2.069 Šin LiFEA to 4.367 Šin LiETFSI. This alteration enhances ionic separation, achieves a more balanced DN, and tunes the self-cleaning intensity for a reinforced SEI. Consequently, the fast charging/discharging capability of LMBs is progressively improved. This rationally tuned anion chemistry reshapes the interactions among Li+, anions, and solvents, presenting new prospects for advanced LMBs.

Entropy-Assisted Anion-Reinforced Solvation Structure for Fast-Charging Sodium-Ion Full Batteries.

Anion-reinforced solvation structure favors the formation of inorganic-rich robust electrode-electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique solvation structure inevitably injures the ionic conductivity of electrolytes and limits the fast-charging performance. Herein, a trade-off in tuning anion-reinforced solvation structure and high ionic conductivity is realized by the entropy-assisted hybrid ester-ether electrolyte. Anion-reinforced solvation sheath with more anions occupying the inner Na+ shell is constructed by introducing the weakly coordinated ether tetrahydrofuran into the commonly used ester-based electrolyte, which merits the accelerated desolvation energy and gradient inorganic-rich electrode-electrolyte interface. The improved ionic conductivity is attributed to the weakly diverse solvation structures induced by entropy effect. These enable the enhanced rate performance and cycling stability of Prussian blue||hard carbon full cells with high electrode mass loading. More importantly, the practical application of the designed electrolyte was further demonstrated by industry-level 18650 cylindrical cells.

Topological Insulator Bi2 Se3 -Assisted Heterostructure for Ultrafast Charging Sodium-Ion Batteries.

The development of fast charging materials offers a viable solution for large-scale and sustainable energy storage needs. However, it remains a critical challenge to improve the electrical and ionic conductivity for better performance. Topological insulator (TI), a topological quantum material that has attracted worldwide attention, hosts unusual metallic surface states and consequent high carrier mobility. Nevertheless, its potential in promising high-rate charging capability has not been fully realized and explored. Herein, a novel Bi2 Se3 -ZnSe heterostructure as excellent fast charging material for Na+ storage is reported. Ultrathin Bi2 Se3 nanoplates with rich TI metallic surfaces are introduced as an electronic platform inside the material, which greatly reduces the charge transfer resistance and improves the overall electrical conductivity. Meanwhile, the abundant crystalline interfaces between these two selenides promote Na+ migration and provide additional active sites as well. As expected, the composite delivers the excellent high-rate performance of 360.5 mAh g-1 at 20 A g-1 and maintains its electrochemical stability of 318.4 mAh g-1 after 3000 long cycles, which is the record high for all reported selenide-based anodes. This work is anticipated to provide alternative strategies for further exploration of topological insulators and advanced heterostructures.

Superior Rate Capability of Small Regenerated Graphite Particles Induced by Homogeneously Distributed Current Density Derived from Cracks and Intrinsic Defects.

As spent batteries can be considered as alternative raw sources of electrode materials; the development of regeneration techniques for spent graphite becomes key to realizing economic and environmental sustainability. Herein, the reutilization of small spent graphite particles is domonstrated due to their special structural characteristics, which may directly contribute to the improvement of lithiation kinetics and high-rate charging during long-term cycling. Such intrinsic defects and external cracked channels may be introduced by the aging of intrinsic bulk structure and exfoliation of surface structure. On account of these potential advantages, a carbonized polypyrrole layer on sieved small graphite particles is developed to obtain superior rate performance. The coated amorphous/graphitic layer could repair the exposed edge and basal plane, and significantly facilitate Li ion diffusion during fast charging. Moreover, the enhanced performance may favor the improved homogeneity of current density distribution during fast charging, which is confirmed by a porous electrode model. The regenerated graphite with a disorder/order coating layer could effectively regulate the Li+ transport channel, exhibiting a high specific capacity at high-rate charging (102.7 mAh g-1 at 4 C after 500 cycles) without severe Li plating. This work provides an opportunity to utilize spent graphite in fast-charging batteries.

2D Layered Materials for Fast-Charging Lithium-Ion Battery Anodes.

The development of electric vehicles has received worldwide attention in the background of reducing carbon emissions, wherein lithium-ion batteries (LIBs) become the primary energy supply systems. However, commercial graphite-based anodes in LIBs currently confront significant difficulty in enduring ultrahigh power input due to the slow Li+ transport rate and the low intercalation potential. This will, in turn, cause dramatic capacity decay and lithium plating. The 2D layered materials (2DLMs) recently emerge as new fast-charging anodes and hold huge promise for resolving the problems owing to the synergistic effect of a lower Li+ diffusion barrier, a proper Li+ intercalation potential, and a higher theoretical specific capacity with using them. In this review, the background and fundamentals of fast-charging for LIBs are first introduced. Then the research progress recently made for 2DLMs used for fast-charging anodes are elaborated and discussed. Some emerging research directions in this field with a short outlook on future studies are further discussed.

Fast and Durable Lithium Storage Enabled by Tuning Entropy in Wadsley-Roth Phase Titanium Niobium Oxides.

Wadsley-Roth phase titanium niobium oxides have received considerable interest as anodes for lithium ion batteries. However, the volume expansion and sluggish ion/electron transport kinetics retard its application in grid scale. Here, fast and durable lithium storage in entropy-stabilized Fe0.4 Ti1.6 Nb10 O28.8 (FTNO) is enabled by tuning entropy via Fe substitution. By increasing the entropy, a reduction of the calcination temperature to form a phase pure material is achieved, leading to a reduced grain size and, therefore, a shortening of Li+ pathway along the diffusion channels. Furthermore, in situ X-ray diffraction reveals that the increased entropy leads to the decreased expansion along a-axis, which stabilizes the lithium intercalation channel. Density functional theory modeling indicates the origin to be the more stable FeO bond as compared to TiO bond. As a result, the rate performance is significantly enhanced exhibiting a reversible capacity of 73.7 mAh g-1 at 50 C for FTNO as compared to 37.9 mAh g-1 for its TNO counterpart. Besides, durable cycling is achieved by FTNO, which delivers a discharge capacity of 130.0 mAh g-1 after 6000 cycles at 10 C. Finally, the potential impact for practical application of FTNO anodes has been demonstrated by successfully constructing fast charging and stable LiFePO4 ‖FTNO full cells.

Amorphous Vanadium Oxide Nanosheets with Alterable Polyhedron Configuration for Fast-Charging Lithium-Ion Batteries.

Transition metal oxides with high theoretical capacities are promising anode materials for lithium-ion batteries (LIBs). However, the sluggish reaction kinetics remain a bottleneck for fast-charging applications due to its slow Li+ migration rate. Herein, a strategy is reported of significantly reducing the Li+ diffusion barrier of amorphous vanadium oxide by constructing a specific ratio of the VO local polyhedron configuration in amorphous nanosheets. The optimized amorphous vanadium oxide nanosheets with a ratio ≈1:4 for octahedron sites (Oh ) to pyramidal sites (C4v ) revealed by Raman spectroscopy and X-ray absorption spectroscopy (XAS) demonstrate the highest rate capability (356.7 mA h g-1 at 10.0 A g-1 ) and long-term cycling life (455.6 mA h g-1 at 2.0 A g-1 over 1200 cycles). Density functional theory (DFT)calculations further verify that the local structure (Oh :C4v = 1:4) intrinsically changes the degree of orbital hybridization between V and O atoms and contributes to a higher intensity of electron occupied states near the Fermi level, thus resulting in a low Li+ diffusion barrier for favorable Li+ transport kinetics. Moreover, the amorphous vanadium oxide nanosheets possess a reversible VO vibration mode and volume expansion rate close to 0.3%, as determined through in situ Raman and in situ transmission electron microscopy.