In-situ Ti4+-doped modification of layer-structured Ni-rich LiNi0.83Co0.11Mn0.06O2 cathode materials for high-energy lithium-ion batteries.

The further commercialization of layer-structured Ni-rich LiNi0.83Co0.11Mn0.06O2 (NCM83) cathode for high-energy lithium-ion batteries (LIBs) has been challenged by severe capacity decay and thermal instability owing to the microcracks and harmful phase transitions. Herein, Ti4+-doped NCM83 cathode materials are rationally designed via a simple and low-cost in-situ modification method to improve the crystal structure and electrode-electrolyte interface stability by inhibiting irreversible polarizations and harmful phase transitions of the NCM83 cathode materials due to Ti4+-doped forms stronger metal-O bonds and a stable bulk structural. In addition, the optimal doping amount of the composite cathode material is also determined through the results of physical characterization and electrochemical performance testing. The optimized Ti4+-doped NCM83 cathode material presents wider Li+ ions diffusion channels (c = 14.1687 Å), lower Li+/Ni2+ mixing degree (2.68 %), and compact bulk structure. The cell assembled with the optimized Ti4+-doped NCM83 cathode material exhibits remarkable capacity retention ratio of 95.4 % after 100cycles at 2.0C and room temperature, and outstanding reversible discharge specific capacity of 148.2 mAh g-1 at 5.0C. Even under elevated temperature of 60 °C, it delivers excellent capacity retention ratio of 92.2 % after 100cycles at 2.0C, which is significantly superior to the 47.9 % of the unmodified cathode material. Thus, the in-situ Ti4+-doped strategy presents superior advantages in enhancing the structural stability of Ni-rich cathode materials for LIBs.

Empowering lithium-ion storage: unveiling the superior performance of niobium-based oxide/perovskite heterojunction with built-in electric field.

The increasing demand for high-performance electrode materials in lithium-ion batteries has driven significant attention towards Nb2O5 due to its high working voltage, large theoretical capacity, environmental friendliness, and cost-effectiveness. However, inherent drawbacks such as poor electrical conductivity and sluggish electrochemical reaction kinetics have hindered its lithium storage performance. In this study, we introduced KCa2Nb3O10 into Nb2O5 to form a heterojunction, creating a built-in electric field to enhance the migration and diffusion of Li+, effectively promoting electrochemical reaction kinetics. Under the regulation of the built-in electric field, the charge transfer resistance of the KCa2Nb3O10/Nb2O5 anode decreased by 3.4 times compared to pure Nb2O5, and the Li+ diffusion coefficient improved by two orders of magnitude. Specifically, the KCa2Nb3O10/Nb2O5 anode exhibited a high capacity of 276 mAh g-1 under 1 C, retaining a capacity of 128 mAh g-1 even at 100 C. After 3000 cycles at 25 C, the capacity degradation was only 0.012% per cycle. Through combined theoretical calculations and experimental validation, it was found that the built-in electric field induced by the heterojunction interface contributed to an asymmetric charge distribution, thereby improving the rates of charge and ion migration within the electrode, ultimately enhancing the electrochemical performance of the electrode material. This study provides an effective approach for the rational design of high-performance electrode materials.

Recent progress of flexible rechargeable batteries.

The rapid popularization of wearable electronics, soft robots and implanted medical devices has stimulated extensive research in flexible batteries, which are bendable, foldable, knittable, wearable, and/or stretchable. Benefiting from these distinct characteristics, flexible batteries can be seamlessly integrated into various wearable/implantable devices, such as smart home systems, flexible displays, and implantable sensors. In contrast to conventional lithium-ion batteries necessitating the incorporation of stringent current collectors and packaging layers that are typically rigid, flexible batteries require the flexibility of each component to accommodate diverse shapes or sizes. Accordingly, significant advancements have been achieved in the development of flexible electrodes, current collectors, electrolytes, and flexible structures to uphold superior electrochemical performance and exceptional flexibility. In this review, typical structures of flexible batteries are firstly introduced and classified into mono-dimensional, two-dimensional, and three-dimensional structures according to their configurations. Subsequently, five distinct types of flexible batteries, including flexible lithium-ion batteries, flexible sodium-ion batteries, flexible zinc-ion batteries, flexible lithium/sodium-air batteries, and flexible zinc/magnesium-air batteries, are discussed in detail according to their configurations, respectively. Meanwhile, related comprehensive analysis is introduced to delve into the fundamental design principles pertaining to electrodes, electrolytes, current collectors, and integrated structures for various flexible batteries. Finally, the developments and challenges of flexible batteries are summarized, offering viable guidelines to promote the practical applications in the future.

Remaining useful life prediction of high-capacity lithium-ion batteries based on incremental capacity analysis and Gaussian kernel function optimization.

Remaining useful life (RUL) is a key indicator for assessing the health status of lithium (Li)-ion batteries, and realizing accurate and reliable RUL prediction is crucial for the proper operation of battery systems. As high-capacity Li batteries have more complex chemical properties, most of the current RUL prediction methods rely mainly on a priori knowledge to make judgments. As a result, prediction accuracy is not high. In this study, we developed a health indicator-capacity (HI-C) dual Gaussian process regression (GPR) model based on incremental capacity analysis (ICA) and optimized its kernel function to achieve accurate RUL prediction for 280 Ah high-capacity Li batteries. Validation against the United States National Aeronautics and Space Administration's four battery test datasets showed that the use of the HI-C dual GPR model resulted in a mean absolute percentage error and root mean square error of less than 0.02 and 0.04, respectively, for the four battery-rated capacity predictions. Additionally, this model achieved an absolute error of less than five battery failure turns. Compared with a single model, the HI-C dual GPR model not only had high accuracy but also solved the problem that the HI was not measurable in the actual battery operation, which made it more suitable for RUL prediction of Li batteries.

Exploring the Mechanisms of LiNiO2 Cathode Degradation by the Electrolyte Interfacial Deprotonation Reaction.

Nickel-rich layered oxides stand as ideal cathode candidates for high specific capacity and energy density next-generation lithium-ion batteries. However, increasing the Ni content significantly exacerbates structural degradation under high operating voltage, which greatly restricts large-scale commercialization. While strategies are being developed to improve cathode material stability, little is known about the effects of electrolyte-electrode interaction on the structural changes of cathode materials. Here, using LiNiO2 in contact with electrolytes with different proton-generating levels as model systems, we present a holistic picture of proton-induced structural degradation of LiNiO2. Through ab initio molecular dynamics calculations based on density functional theory, we investigated the mechanisms of electrolyte deprotonation, protonation-induced Ni dissolution, and cathode degradation and the impacts of dissolved Ni on the Li metal anode surfaces. We show that the proton-transfer reaction from electrolytes to cathode surfaces leads to dissolution of Ni cations in the form of NiOOHx, which stimulates cation mixing and oxygen loss in the lattice accelerating its layered-spinel-rock-salt phase transition. Migration of dissolved Ni2+ ions to the anode side causes their reduction into the metallic state and surface deposition. This work reveals that interactions between the electrolyte and cathode that result in protonation can be a dominant factor for the structural stability of Ni-rich cathodes. Considering this factor in electrolyte design should be of benefit for the development of future batteries.

Cross-Scale Decoupling Kinetic Processes in Lithium-Ion Batteries Using the Multi-Dimensional Distribution of Relaxation Time.

To non-destructively resolve and diagnose the degradation mechanisms of lithium-ion batteries (LIBs), it is necessary to cross-scale decouple complex kinetic processes through the distribution of relaxation times (DRT). However, LIBs with low interfacial impedance render DRT unreliable without data processing and closed-loop validation. This study proposes a hierarchical analytical framework to enhance timescale resolution and reduce uncertainty, including interfacial impedance reconstruction and multi-dimensional DRT analysis. Interfacial impedance is reconstructed by eliminating simulated inductive and diffusive impedance based on a high-fidelity frequency-domain model. Multi-dimensional DRT decouples solid electrolyte interphase (SEI) and charge transfer (CT) processes by the reversibility of electrochemical reactions with state of charge (SOC) to characterize electrode kinetic evolution driven by SOC and temperature through timescales and peak area. The findings reveal that reconstructed impedance improves the accuracy of identified time constants by ≈20%. Cross-scale DRT results reveal that SOCs below 10% at 25 °C effectively distinguish electrode kinetics due to the high correlation between cathodic CT and SOC. Kinetic metrics characterize that anodic SEI or CT are different control steps limiting the low-temperature performance of different cells. This work underscores the potential of the proposed framework for non-destructive diagnostics of kinetic evolution.

Artificial Electron Channels Enable Contact Prelithiation of Li-Ion Battery Anodes with Ultrahigh Li-Source Utilization.

Contact prelithiation is widely used for compensating the initial capacity loss of lithium-ion batteries (LIBs). However, the low Li-source utilization suffering from the deteriorated contact interfaces results in cycling degeneration. Herein, Li-Ag alloy-based artificial electron channels (AECs) are established in Li source/graphite anode contact interfaces to promote Li-source conversion. Due to the shielding effect of the Li-Ag alloy (50 at. % Li) on Li-ion diffusion, the dry-state corrosion of contact interfaces is restricted. The unblocked electronic conduction across the AEC-involved interface not only facilitates the Li source conversion but also accelerates the prelithiation kinetics during the wet-state process, resulting in an ultrahigh Li-source utilization (90.7%). Thereby, implementing AEC-assisted prelithiation in a LiNi0.5Co0.2Mn0.3O2 pouch cell yields a 35.8% increase in energy density and stable cycling over 600 cycles. This finding affords significant insights into the construction of an efficient prelithiation technology toward the development of high-energy LIBs.

Reductive Dissolution of NCM Cathode through Anaerobic Respiration by Shewanella putrefaciens.

The consumption of lithium-ion batteries (LIBs) has considerably increased over the past decade, leading to a rapid increase in the number of spent LIBs. Exposing spent LIBs to the environment can cause serious environmental harm; however, there is a lack of experimentally obtained information regarding the environmental impacts of abandoned cathode materials. Here, we report the interactions between Shewanella putrefaciens, a microorganism commonly found in diverse low-oxygen natural settings, and LiNi0.6Co0.2Mn0.2O2 (NCM622) under anaerobic conditions. We present compelling evidence that the anaerobic respiration of Shewanella putrefaciens triggers ∼59 and ∼78% dissolution of 0.2 g/L pristine and spent NCM622, respectively. We observed that Shewanella putrefaciens interacted with the pristine and the spent NCM622 under anaerobic conditions at a neutral pH and room temperature and induced the reduction of Ni, Co, and Mn, resulting in the subsequent dissolution of Li, Ni, Co, and Mn. Moreover, we found that secondary mineralization occurred on the surface of reacted NCM622. These findings not only shed light on the substantial impact of microbial respiration on the fate of discarded cathode materials in anaerobic environments but also reveal the potential for sustainable bioleaching of cathodes in spent LIBs.

Selective Methylation of Cyclic Ether Towards Highly Elastic Solid Electrolyte Interphase for Silicon-based Anodes.

Silicon (Si)-based anodes offer high theoretical capacity for lithium-ion batteries but suffer from severe volume changes and continuous solid electrolyte interphase (SEI) degradation. Here, we address these challenges by selective methylation of 1,3-dioxolane (DOL), thus shifting the unstable bulk polymerization to controlled interfacial reactions and resulting in a highly elastic SEI. Comparative studies of 2-methyl-1,3-dioxolane (2MDOL) and 4-methyl-1,3-dioxolane (4MDOL) reveal that 4MDOL, with its larger ring strain and more stable radical intermediates due to hyperconjugation effect, promotes the formation of high-molecular-weight polymeric species at the electrode-electrolyte interface. This elastic, polymer-rich SEI effectively accommodates volume changes of Si and inhibits continuous side reactions. Our designed electrolyte enables Si-based anode to achieve 85.4% capacity retention after 400 cycles at 0.5 C without additives, significantly outperforming conventional carbonate-based electrolytes. Full cells also demonstrate stable long-term cycling. This work provides new insights into molecular-level electrolyte design for high-performance Si anodes, offering a promising pathway toward next-generation lithium-ion batteries with enhanced energy density and longevity.

Dramatic Enhancement Enabled by Introducing TiN into Bread-like Porous Si-Carbon Anodes for High-Performance and Safe Lithium Storage.

Doping modifications and surface coatings are effective methods to slow volume dilatation and boost the conductivity in silicon (Si) anodes for lithium-ion batteries (LIBs). Herein, using low-cost ferrosilicon from industrial production as the energy storage material, a bread-like nitrogen-doped carbon shell-coated porous Si embedded with the titanium nitride (TiN) nanoparticle composite (PSi/TiN@NC) was synthesized by simple ball milling, etching, and self-assembly growth processes. Remarkably, the porous Si structure formed by etching the FeSi2 phase in ferrosilicon alloys can provide buffer space for significant volume expansion during lithiation. Highly conductive and stable TiN particles can act as stress absorption sites for Si and improve the electronic conductivity of the material. Furthermore, the nitrogen-doped porous carbon shell further helps to sustain the structural stability of the electrode material and boost the migration rate of Li-ions. Benefiting from its unique synergistic effect of components, the PSi/TiN@NC anode exhibits a reversible discharge capacity up to 1324.2 mAh g-1 with a capacity retention rate of 91.5% after 100 cycles at 0.5 A g-1 (vs fourth discharge). Simultaneously, the electrode also delivers good rate performance and a stable discharge capacity of 923.6 mAh g-1 over 300 cycles. This research can offer a potential economic strategy for the development of high-performance and inexpensive Si-based anodes for LIBs.

A Fast Self-Healing Binder for Highly Stable SiOx Anodes in Lithium-Ion Batteries.

Silicon oxide-based (SiOx-based) materials show great promise as anodes for high-energy lithium-ion batteries due to their high specific capacity. However, their practical application is hindered by the inevitable volumetric expansion during the lithiation/delithiation process. Constructing high-performance binders for SiOx-based anodes has been regarded as an efficient strategy to mitigate their volume expansion and preserve structural integrity. In this work, we propose a green water-solution PAA-LS binder composed of poly(acrylic acid) (PAA) and sodium lignosulfonate (LS) with fast self-healing properties. The designed binder can be restored due to the strong affinity between Fe3+-catechol coordination bonds, thereby effectively alleviating the volumetric strain of SiOx-based anodes. Notably, with an optimized LS content of 0.5%, the SiOx@PAA-LS electrode exhibits excellent performance, delivering a high capacity of 997.3 mAh g-1 after 450 cycles at 0.5 A g-1. Furthermore, the SiOx||NCM622 full cell also demonstrates superior cycling stability, maintaining a discharge capacity of 147.58 mAh g-1 after 100 cycles at 0.5 A g-1, with an impressive capacity retention rate of 82.72%.

Promoting nitrogen-doped porous phosphorus spheres for high-rate lithium storage.

Phosphorus anode has shown great potential for the high-rate and high-energy-density lithium-ion batteries. Nevertheless, it still suffers from possible electrode cracking, ion-transport restrictions, and active-particle decomposition resulting from repeated alloying/de-alloying. To address the aforementioned issues, a nitrogen-doped flower-like porous phosphorus (f-P) sphere has been developed. The abundant micro-mesopores facilitate ion diffusion and enhance the internal bonding strength of the electrode. Concurrently, the doped nitrogen promotes the generation of a favorable solid electrolyte interphase constructed by fast-ion-conductors. As a result, the f-P exhibits a high-rate capacity of 735mAh g-1 at 20 A g-1 and maintains high Coulombic efficiencies over 900 cycles at 10 A g-1. Furthermore, coin full-cells comprising the f-P anode and lithium cobalt oxide cathode demonstrate stable operation at a high current density of 6 mA cm-2. The combination of a porous structure and doping strategy represents a viable approach for strengthening the durability of electrodes and optimizing the ion transport kinetics of advanced alloy anode materials.

Defect-Mediated Formation of Oriented Phase Domains in a Lithium-Ion Insertion Electrode.

The performance and robustness of electrodes are closely related to transformation-induced nanoscale structural heterogeneity during (de)lithiation. As a result, it is critical to understand at atomic scale the origin of such structural heterogeneity and ultimately control the transformation microstructure, which remains a formidable task. Here, by performing in situ studies on a model intercalation electrode material, anatase TiO2, we reveal that defects─both preexisting and as-formed during lithiation─can mediate the local anisotropic volume expansion direction, resulting in the formation of multiple differently oriented phase domains and eventually a network structure within the lithiated matrix. Our results indicate that such a mechanism operated by defects, if properly harnessed, could not only improve lithium transport kinetics but also facilitate strain accommodation and mitigate chemomechanical degradation. These findings provide insights into the connection of defects to the robustness and rate performance of electrodes, which help guide the development of advanced lithium-ion batteries via defect engineering.

Concisely Constructing S, F Co-Modified MnO Nanoparticles Attached to S, N Co-Doped Carbon Skeleton as a High-Rate Performance Anode Material.

The utilization of MnO anodes with high storage capacity is significantly hindered by rapid capacity fading and inadequate rate capability, stemming from substantial volume fluctuations and low electrical conductivity. Crafting a composite comprising sulfur and fluorine co-modified MnO nanoparticles integrated with sulfur and nitrogen co-doped carbon matrices promises enhanced electrochemical performance yet poses formidable obstacles. Here, we present a straightforward synthetic strategy for in situ growth of sulfur and fluorine co-modified MnO nanoparticles onto sulfur and nitrogen co-doped carbon scaffolds. This integration effectively mitigates volume variations and enhances electrical conductivity. As a result, the SF-MnO/SNC composite demonstrates remarkable cycling stability and rate capability when employed as a lithium-ion battery anode. Remarkably, it achieves a high reversible capacity of 975 mAh g-¹ after 80 cycles at 0.1 A g-¹ and retains a substantial capacity of 498 mAh g-¹ even at a high rate of 2.0 A g-¹. The concise synthesis method and exceptional rate properties render the SF-MnO/SNC composite a promising anode material for lithium-ion batteries. The strategy of simultaneously doping oxides and carbon will bring new ideas to the research of oxide anodes.

Unveiling the Influences of In Situ Carbon Content on the Structure and Electrochemical Properties of MoS2/C Composites.

In this work, a MoS2/C heterostructure was designed and prepared through an in situ composite method. The introduction of carbon during the synthesis process altered the morphology and size of MoS2, resulting in a reduction in the size of the flower-like structures. Further, by varying the carbon content, a series of characterization methods were employed to study the structure and electrochemical lithium storage performance of the composites, revealing the effect of carbon content on the morphology, structure characteristics, and electrochemical performance of MoS2/C composites. The experimental setup included three sample groups: MCS, MCM, and MCL, with glucose additions of 0.24 g, 0.48 g, and 0.96 g, respectively. With increasing carbon content, the size of MoS2 initially decreases, then increases. Among these, the MCM sample exhibits the optimal structure, characterized by smaller MoS2 dimensions with less variation. The electrochemical results showed that MCM exhibited excellent electrochemical lithium storage performance, with reversible specific capacities of 956.8, 767.4, 646.1, and 561.4 mAh/g after 10 cycles at 100, 200, 500, and 1000 mA/g, respectively.

Effect of Sulfur Modification on Structural and Electrochemical Performance of Pitch-Based Carbon Materials for Lithium/Sodium Ion Batteries.

Coal tar pitch (CTP) has become an ideal choice in the preparation of anode precursors for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) because of its abundant carbon content, competitive pricing and adjustable structure properties. In this paper, sulfurized pitch-based carbon (SPC-800) was obtained by allowing CTP to react with sulfur at 350 °C and subsequently achieve carbonization at 800 °C. SPC-800 was more disordered and had a larger layer spacing than carbonized CTP (PC-800). Upon utilization as an anode for LIBs, SPC-800 possessed a higher reversible specific capacity (478.1 mAh g-1 at 0.1 A g-1), while utilization in SIBs displayed a capacity of 220.9 mAh g-1 at 20 mA g-1. This work is an important guide to the design of high-performance anodes suitable for use with both LIBs and SIBs.

Comparative Investigation of Water-Based CMC and LA133 Binders for CuO Anodes in High-Performance Lithium-Ion Batteries.

Transition metal oxides are considered to be highly promising anode materials for high-energy lithium-ion batteries. While carbon matrices have demonstrated effectiveness in enhancing the electrical conductivity and accommodating the volume expansion of transition metal oxide-based anode materials in lithium-ion batteries (LIBs), achieving an optimized utilization ratio remains a challenging obstacle. In this investigation, we have devised a straightforward synthesis approach to fabricate CuO nano powder integrated with carbon matrix. We found that with the use of a sodium carboxymethyl cellulose (CMC) based binder and fluoroethylene carbonate additives, this anode exhibits enhanced performance compared to acrylonitrile multi-copolymer binder (LA133) based electrodes. CuO@CMC electrodes reveal a notable capacity ~1100 mA h g-1 at 100 mA g-1 following 170 cycles, and exhibit prolonged cycling stability, with a capacity of 450 mA h g-1 at current density 300 mA g-1 over 500 cycles. Furthermore, they demonstrated outstanding rate performance and reduced charge transfer resistance. This study offers a viable approach for fabricating electrode materials for next-generation, high energy storage devices.

Free-Standing Poly(vinyl benzoquinone)/Reduced Graphene Oxide Composite Films as a Cathode for Lithium-Ion Batteries.

Quinones with a rapid reduction-oxidation rate are promising high-capacity cathodes for lithium-ion batteries. However, the high solubility of quinone molecules in polar organic electrolytes results in low cycle stability, while their low electric conductivity causes low utilization of electrode materials. In this article, a new p-benzoquinone derivative, poly(vinyl benzoquinone) (PVBQ), is designed and synthesized, and a solution-based method of preparing free-standing PVBQ/reduced graphene oxide (RGO) composite films is developed. PVBQ has a high theoretical specific capacity (400 mA h g-1) because of its low dead moiety mass. In the produced composite films, PVBQ nanoparticles are uniformly dispersed on RGO sheets, which endows the composite films with high electric conductivity and inhibits the dissolution of PVBQ through strong adsorption. As a result, the composite films show a high active material utilization, high practical specific capacity, and excellent cycling stability. PVBQ in the composite membrane containing 60.2 wt % RGO deliver 244 mA h g-1 capacity after 200 charge-discharge cycles at a current density of 300 mA g-1. At a current density of 1500 mA g-1, the reversible specific capacity is still 170 mA h g-1. This work provides a high-performance cathode material for lithium-ion batteries, and the molecular structure and electrode structure design ideas are also instructive for developing other organic electrode materials.

Probing Surface Dynamics of SiOx Thin-Film Electrodes during Cycling through X-Ray Photoemission Spectroscopy and Operando X-Ray Reflectivity.

SiOx electrodes are promising for high-energy-density lithium-ion batteries (LIBs) due to their ability to mitigate volume expansion-induced degradation. Here, we investigate the surface dynamics of SiOx thin-film electrodes cycled in different carbonate-based electrolytes using a combination of ex situ X-ray photoelectron spectroscopy (XPS) and operando synchrotron X-ray reflectivity analyses. The thin-film geometry allows us to probe the depth-dependent chemical composition and electron density from surface to current collector through the solid electrolyte interphase (SEI), the active material, and the thickness evolution during cycling. Results reveal that SiOx lithiation initiates below 0.4 V vs Li+/Li and indicate a close relationship between SEI formation and SiOx electrode lithiation, likely due to the high resistivity of SiOx. We find similar chemical compositions for the SEI in FEC-containing and FEC-free electrolytes but observe a reduced thickness in the former case. In both cases, the SEI thickness decreases during delithiation due to the removal or dissolution of some carbonate species. These findings give insights into the (de)lithiation of SiOx, in particular, during the formation stage, and the effect of the presence of FEC in the electrolyte on the evolution of the SEI during cycling.

Oxygen Self-Doping Bi2S3@C Spheric Successfully Enhanced Long-Term Performance in Lithium-Ion Batteries.

High theoretical capacity of Bi2S3 propels it toward an ideal anode material for lithium-ion batteries (LIBs); however, rapid capacity attenuation and poor long-term stability are major barriers to widespread application. In this work, an oxygen self-doping strategy was utilized to synthesize O-Bi2S3@C, significantly increasing the amount of active sites for lithium-ion storage. Meanwhile, sulfur vacancies were formed to improve the electrical conductivity and ionic transport efficiency, enhance the long-term stability, and accelerate the electrochemical kinetics of Bi2S3@C. O-BSC-S1:3 anode exhibits a reversible capacity of 673.1 mAh g-1 at 0.2 A g-1. It retains a long-term capacity of 596.3 mAh g-1 over 1100 cycles at a high density of 3 A g-1 in LIBs. Moreover, the installed O-Bi2S3@C//LiCoO2 full battery offers exceptional reversible capacity and remarkable cyclability (325.2 mAh g-1 after 200 cycles) at 0.2 A g-1. The combined strategy of oxygen self-doping and sulfur vacancy effectively enhances the reversible capacity and cycling life of Bi2S3, providing an approach for the design of high-performance transition metal sulfide anodes for LIBs.