Lithium Migration Research Articles

Engineering the Hole Transport Layer with a Conductive Donor-Acceptor Covalent Organic Framework for Stable and Efficient Perovskite Solar Cells.

Spiro-OMeTAD doped with lithium-bis(trifluoromethylsulfonyl)-imide (Li-TFSI) and tertbutyl-pyridine (t-BP) is widely used as a hole transport layer (HTL) in n-i-p perovskite solar cells (PSCs). Spiro-OMeTAD based PSCs typically show poor stability owing to the agglomeration of Li-TFSI, the migration of lithium ions (Li+), and the existence of potential mobile defects originating from the perovskite layer. Thus, it is necessary to search for a strategy that suppresses the degradation of PSCs and overcomes the Shockley Queisser efficiency limit via harvesting excess energy from hot charge carrier. Herein, two covalent organic frameworks (COFs) including BPTA-TAPD-COF and a well-defined donor-acceptor COF (BPTA-TAPD-COF@TCNQ) were developed and incorporated into Spiro-OMeTAD HTL. BPTA-TAPD-COF and BPTA-TAPD-COF@TCNQ could act as multifunctional additives of Spiro-OMeTAD HTL, which improve the photovoltaic performance and stability of the PSC device by accelerating charge-carrier extraction, suppressing the Li+ migration and Li-TFSI agglomeration, and capturing mobile defects. Benefiting from the increased conductivity, the addition of BPTA-TAPD-COF@TCNQ in the device led to the highest power conversion efficiency of 24.68% with long-term stability in harsh conditions. This work provides an example of using COFs as additives of HTL to enable improvements of both efficiency and stability for PSCs.

Analysis of polyanion single ion conductor based on preparation of gel electrolyte for lithium ion battery

Abstract This study achieved efficient preparation of polyanionic single ion conductors by selecting appropriate raw materials and controlling preparation conditions. The results show that the window stability of electrolytic gel with a wide ionic electrochemical conductor is 2-4.5 V and 0.74 lithium ion migration. Lithium iron phosphate battery (LFP) is the positive electrode, lithium metal is the negative electrode, and PVDF-HFP Pampsli ion is the electrolyte. When lithium salt is not added, the rated power of the battery is 125 mah·g-1, and the current density is 2 C. The battery has a range of more than 500 times. In the current high-density 5 C situation, it has a specific capacity of 100 mAh·g-1 and a stable cycling ability of over 300 cycles, while maintaining nearly 100% stable Colomb efficiency.

Voltage Control of Multiple Electrochemical Processes during Lithium Ion Migration in NiFe2O4 Ferrite.

Li-ion-based electric field control has been attracting significant attention, since it is able to penetrate deep into materials to exhibit diverse and controllable electrochemical processes, which offer more degrees of freedom to design multifunctional devices with low power consumption. As opposed to previous studies that mainly focused on single lithiation/delithiation mechanisms, we reveal three Li-ion modulation mechanisms in the same NiFe2O4 spinel ferrite by in situ magnetometry, i.e., intercalation, conversion, and space charge, which are respectively demonstrated in high, medium, and low voltage range. During the intercalation stage, the spinel structure is preserved, and a reversible modulation of magnetization arises from the charge transfer-induced variation of Fe valence states (Fe2+/Fe3+). Conversion-driven change in magnetization is the largest up to 89 emu g-1, due to the structural and magnetic phase transitions. Although both intercalation and conversion exhibit sluggish kinetics and long response times, the space charge manifests a faster switching speed and superior durability due to its interface electrostatic effect. These results not only provide a clear and comprehensive understanding on Li-based modulation mechanisms but also facilitate multifunctional and multiscenario applications, such as multistate memory, micromagnetic actuation, artificial synapse, and energy storage.

Multiphase transformation and mechanical analysis of polycrystalline [formula omitted] nanoparticle during lithiation via phase diagram-guided phase-field approach

The fabrication of tin (Sn)-based materials with exceptional electrochemical and mechanical properties requires a thorough understanding of the multiphase evolution that occurs during lithiation. However, predicting the microstructural changes during this process using analytical models is challenging due to the intricate interactions among electrode materials, cell operating parameters, complex geometries, and polycrystalline structures. To tackle this challenge, we propose the application of the phase-field method in a grand-potential formulation, that is combined with the smooth boundary method to apply constant-current (de-)lithiation boundary conditions. This approach effectively describes the migration of lithium and the multiphase transitions in polycrystalline electrodes with arbitrary geometries. To investigate nanoparticles with hundreds of grains in two/three dimensions efficiently, we have incorporated this model into the self-developed open-source phase-field solver package MInDes in a highly optimized manner. Further, comparing the output voltage of the simulated lithiation process of LixSn nanoparticles in three dimensions demonstrates an excellent correlation with experimental results. Based on this, we analyze the mechanical performance of polycrystalline nanoparticles with varying amounts of copper doping and evaluate the maximal von Mises stress during lithiation to predict the onset of crack formation.

Evolution of the Electrical Conductivity of LiNb1−xTaxO3 Solid Solutions across the Ferroelectric Phase Transformation

The investigation of the structural phase transition in the vicinity of the Curie temperature of crystals is motivated by the expected combination of advantageous high‐temperature properties of and , including high piezoelectric modules and remarkable high‐temperature stability, respectively. marks the ultimate limit for exploiting the piezoelectric properties; however, transition‐related structural modifications might impact this and other properties even below . Remarkably, the phase transition from the ferroelectric to the paraelectric phase, whose temperature strongly depends on the composition x, shows a significant drop in the activation energy of the electrical conductivity. The magnitude, temperature dependence, and underlying mechanisms of this drop are discussed from a microscopic perspective. Molecular dynamics calculations in the framework of the density functional theory show that substantial displacements of the cations occur below for both the end compounds and , and might thus affect the electrical conductivity. Above , the migration of lithium ions is presumably facilitated by a shortened diffusion path for the most favorable jump of the lithium ions. Electronic contributions to the conductivity, which become important above 900 K, are explained within the polaronic picture by the formation and migration of free small polarons.

Building Flame-Retardant Polymer Electrolytes via Microcapsule Technology for Stable Lithium Batteries.

Flame retardants could improve the safety properties of lithium batteries (LBs) with the sacrifice of electrochemical performance due to parasitic reactions. To concur with this, we designed thermal-response clothes for hexachlorophosphazene (HCP) additives by the microcapsule technique with urea-formaldehyde (UF) resin as the shell. HCP@UF combines with polyacrylonitrile (PAN) by hydrogen bonds successfully to form PAN-HCP@UF as the flame-retardant solid polymer electrolyte. The hydrogen bonds ensure excellent mechanical properties of the polymer electrolyte. The multiscale free radical-annihilating agent HCP effectively eliminates hydrogen free radicals of electrolytes under high temperature, showing excellent flame retardation. During the operation of the battery, functional groups on the UF resin act as active sites to promote the migration of lithium ions, while the internal HCP is protected from electrochemical reaction. With 25% HCP@UF addition, the limiting oxygen index of the PAN-HCP@UF increases to 28% and the Li+ transfer number up to 0.80. By UF protection, the initial capacity retention rate of the Li||LFP battery that assembles with PAN-HCP@UF is 88.8% after 500 cycles at 0.5 C. Thus, the microcapsule-encapsulated approach is deemed to provide an innovative strategy to prepare high-safety solid-state LB with a stable long cycle life.

Effect of hydroxy-terminated hyperbranched polymer coated separator on the lithium-ion battery performances

Abstract The hydrophobicity of polyolefin separators causes poor compatibility with the internal environment of lithium-ion batteries and thus elevates lithium-ion migration barriers. In this research, hydroxy-terminated hyperbranched polymer (HTHP) coated separators are fabricated successfully based on the simple and easy-on impregnation method. Abundant hydroxyl groups in HTHP reinforce separator electrolyte affinity, generating the much lower contact angle and higher electrolyte uptake. Accordingly, HTHP-coated separators show broader electrochemical window and superior ionic conductivity and Li+ transport number, which facilitate the Li+ migration within porous pathways and hence maximally weaken counteranions-induced polarizations. The lower interfacial resistances also guarantee the Li+ accelerated diffusion via the separator–electrodes interfaces. Therefore, batteries containing modified separators exhibit optimized C-rate capacity and cycling stability. However, immoderate HTHP coating blocks partial pores and thus restricts Li+ transference, which deteriorates C-rate capacity and cycling durability in turn. This separator modification scheme possesses advantages of simple preparation, environment-friendly, and low manufacturing cost, providing practical guidance for low-cost and high-performance separator manufacture.

Two-dimensional phthalocyanine-based molecular additives realize efficient hole transport and enhanced ion immobilization for durable perovskite solar cells

Perovskite solar cells (PSCs) have demonstrated high promises in low-cost manufacture and outstanding power conversion efficiencies (PCEs), however, long-term operational stability has become the major obstacle challenging the scalable application of this technology. Although the state-of-the-art hole transport layer (HTL) based on Spiro-OMeTAD becomes the indispensable component in high-efficiency PSCs, the dopants in the HTLs cause severe stability issues of ion migration and phase segregation, all of which induce the degradation of HTLs in the aspects of film conductivity and microstructures. Here we rationally design a two-dimensional phthalocyanine-based molecular additive (TB-C8-Ni) for the HTLs in order to enhance the carrier transportation and immobilize the ions. The incorporation of [8-(4-tert-butylphenoxy)octyl]oxy alkyl units as the side groups in TB-C8-Ni is essential to increase the solubility and improve the HTL uniformity. The superior planar structure of TB-C8-Ni favors the hole transportation and suppresses the migration of lithium ion under the environmental stress, which achieves reliable HTLs and devices. Consequently, the devices based on TB-C8-Ni exhibit boosted open-circuit voltage and fill factor, delivering an increased efficiency from 20.93% to 22.34%. More importantly, the additive TB-C8-Ni in the HTLs reinforces the moisture stability of devices, enabling to maintain 90% of initial efficiency after 2300 h in air.

Construction of greenly biodegradable bacterial cellulose/UiO-66-NH2 composite separators for efficient enhancing performance of lithium-ion battery

The disposal of waste lithium batteries, especially waste separators, has always been a problem, incineration and burial will cause environmental pollution, therefore, the development of degradable and high-performance separators has become an important challenge. Herein, UiO-66-NH2 particles were successfully anchored onto bacterial cellulose (BC) separators by epichlorohydrin (ECH) as a crosslinker, then a BC/UiO-66-NH2 composite separator was prepared by vacuum filtration. The ammonia groups (−NH2) from UiO-66-NH2 can form hydrogen bonds with PF6− in the electrolyte, promoting lithium-ion transference. Additionally, UiO-66-NH2 can store the electrolyte and tune the porosity of the separator. The lithium ion migration number (0.62) of the battery assembled with BC/UiO-66-NH2 composite separator increased by 50 % compared to the battery assembled with commercial PP separator (0.45). The discharge specific capacity of the battery assembled with BC/UIO-66-NH2 composite separator after 50 charge and discharge cycles is 145.4 mAh/g, which is higher than the average discharge specific capacity of 114.3 mAh/g of the battery assembled with PP separator. When the current density is 2C, the minimum discharge capacity of the battery assembled with BC/UiO-66-NH2 composite separator is 85.3 mAh/g. The electrochemical performance of the BC/UiO-66-NH2 composite separator is significantly better than that of the commercial PP separator. In addition, -NH2 can offer a nitrogen source to facilitate degradation of the BC separators, whereby the BC/UiO-66-NH2 composite separator could be completely degraded in 15 days.

Research on the in-situ flocculation behavior of polyferric silicate for enhancing the lithium leachability in lithium-rich clay

The expansion of global lithium demand urgently requires efficient extraction technologies for lithium-rich clay recourse. However, the encapsulation of polysilicate products in the acidic leaching system impedes the migration of lithium from the mineral to the solution, resulting in a low recovery rate of lithium. Here, this study proposes an in-situ flocculation mechanism of Fe3+ on the polysilicate to reconstruct the surface structure, enhancing the leaching efficiency of lithium. Results showed that the flocculation of Fe3+ approaches the Si-O surface and reacts with silicate to form the polyferric silicate (Fe3Si2O5(OH)4). This special configuration eliminates the wrapping and adsorption effect of polysilicate while promotes the diffusion of Li+. Increased FeCl3 concentration and higher leaching temperature are beneficial for the leaching efficiency of Li. Under optimized conditions, the Li leaching efficiency in the FeCl3 leaching system reaches up to 92.81 %. This work introduces Fe3+ to overcome the limiting effect of polysilicate during acidic leaching, and affords extraordinary recovery of lithium from clay resources.

SiO2-Decorated-Montmorillonite reinforced Poly(1,3-dioxolane) as a multifunctional solid electrolyte for High-Performance lithium batteries

Solid polymer electrolytes (SPEs) have garnered considerable attention owing to their remarkable flexibility, manufacturability, and cost-effectiveness. However, SPEs are hampered by critical limitations such as inadequate ionic conductivity at room temperature and issues related to lithium-ion migration, which curtail their practical applications. To tackle these challenges, the incorporation of inorganic additives into SPEs is considered as an effective strategy. Montmorillonite (MMT), a typical two-dimensional material, has emerged as an advanced filler for SPEs, displaying increased ionic conductivity, lithium-ion transference, and electrochemical stability. Herein, siliconized-modified montmorillonite (SiO2-MMT) nanosheets are synthesized and incorporated into poly(1,3-dioxolane) (PDOL)-based SPEs, resulting in a multifunctional composite solid electrolyte (CSE). The CSE shows an ionic conductivity as high as 5.58 × 10−4 S cm−1 at 30 °C, with a lithium-ion transference number close to 0.58. Symmetrical Li||Li cells utilizing the CSE exhibits stable performance for over 1200 h at a current density of 0.2 mA cm−2. Additionally, the CSE contributes to the stability of electrolytes, facilitates superior Li+ mobility and uniform deposition, thereby forming a stable solid electrolyte interface (SEI). Density functional theory (DFT) simulation confirms that SiO2-MMT, containing a large number of adsorption sites, facilitated fast reaction kinetics and effective anchoring of lithium polysulfides (LiPSs). As a result, the composite electrolyte is cycled in Lithium-sulfur (Li-S) batteries at 200 mA g−1 and 30 °C for 250 cycles, achieving a high coulombic efficiency (CE > 99.4 %) and a capacity decay rate of 0.15 %. Additionally, when paired with high-voltage Li(Ni0.8Co0.1Mn0.1)O2 (NCM811) cathodes and LiFePO4 (LFP) cathodes, both display excellent electrochemical performance. This research presents a highly promising approach for constructing multifunctional solid electrolytes for high-performance lithium batteries.

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 4C.

SiC substrate-facilitated lithium-ion migration to modulate Kekulé-O graphene

Li-ions-intercalated bilayer graphene (BLG) on a SiC substrate can form Kekulé-O mode graphene (Kekulé-O graphene), which has attracted widespread interest for its demonstration of chiral symmetry breaking in particle physics. However, the Kekulé-O mode cannot be observed at high temperatures, which is still a mystery. In this Letter, the effect of the SiC substrate on the migration of Li-ions within the BLG was investigated by first-principles calculations. Our results show that the SiC substrate can significantly reduce the migration energy barrier of Li-ions at both low and high Li concentration. At saturated Li-ion concentration, due to the presence of SiC substrate, Li-ions only need to cross a very small barrier (0.06 eV) to destroy the Kekulé-O graphene. Therefore, the disappearance of Kekulé-O graphene prepared at high temperatures is attributed to the fast migration of Li-ions. This work provides atomic understanding of the temperature modulation of Kekulé-O graphene.

Enhancement mechanism of the comprehensive performance of all-solid-state polymer electrolytes by halloysite nanotubes: Construction of efficient lithium-ion conduction channels

Considering the current issues with poly(ethylene oxide)-based all-solid-state polymer electrolytes (PEO-ASSPEs) employed in lithium-ion batteries (LIBs), such as low ionic conductivity, low lithium-ion transference number, narrow electrochemical stability window, and poor cyclic stability. This study introduces oxygen-vacancy-rich halloysite nanotubes (HNTs) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) into the PEO matrix to fabricate a flexible composite polymer electrolyte (CPEs) via a solvent-free method. The interaction between HNTs and LiTFSI in the PEO matrix serves to mitigate the ionic solvation effect, increase the number of free lithium-ion, and reduce the lithium-ion migration energy barrier. Additionally, the internal framework formed by the mutual stacking of HNTs reduces the number of entanglements in polymer molecular chains, enhances the mobility of the chains, and generates a continuous interface effect, forming fast lithium-ion transport channels. The CPEs prepared in this study are in conformity with the Vogel-Tammann-Fulcher (VTF) empirical equation. The CPE containing 10 wt% HNTs exhibits a high ionic conductivity (7.15 × 10−4 S cm−1) at 25 °C, a high lithium-ion transference number (0.600), a wide electrochemical stability window (5.5 V), and excellent cyclic performance (capacity retention of 82.02 % after 100 cycles at 0.1C), satisfying the electrochemical performance requirements for ASSPEs in LIBs.

Retarding anion migration for alleviating concentration polarization towards stable polymer lithium-metal batteries

Traditional dual-ion lithium salts have been widely used in solid polymer lithium-metal batteries (LMBs). Nevertheless, concentration polarization caused by uncontrolled migration of free anions has severely caused the growth of lithium dendrites. Although single-ion conductor polymers (SICP) have been developed to reduce concentration polarization, the poor ionic conductivity caused by low carrier concentration limits their application. Herein, a dual-salt quasi-solid polymer electrolyte (QSPE), containing the SICP network as a salt and traditional dual-ion lithium salt, is designed for retarding the movement of free anions and simultaneously providing sufficient effective carriers to alleviate concentration polarization. The dual salt network of this designed QSPE is prepared through in-situ crosslinking copolymerization of SICP monomer, regular ionic conductor, crosslinker with the presence of the dual-ion lithium salt, delivering a high lithium-ion transference number (0.75) and satisfactory ionic conductivity (1.16 × 10−3 S cm−1 at 30 °C). Comprehensive characterizations combined with theoretical calculation demonstrate that polyanions from SICP exerts a potential repulsive effect on the transport of free anions to reduce concentration polarization inhibiting lithium dendrites. As a consequence, the Li||LiFePO4 cell achieves a long-cycle stability for 2000 cycles and a 90% capacity retention at 30 °C. This work provides a new perspective for reducing concentration polarization and simultaneously enabling enough lithium-ions migration for high-performance polymer LMBs.

Cationic cellulose nanofiber solid electrolytes: A pathway to high lithium-ion migration and polysulfide adsorption for lithium-sulfur batteries

Polyethylene oxide (PEO) solid electrolytes, acknowledged for their safety advantages over liquid counterparts, confront inherent challenges, including low ionic conductivity, restricted lithium ion migration, and mechanical fragility, notably pronounced in lithium‑sulfur batteries due to the polysulfide shuttling phenomenon. To address these limitations, we integrate a quaternary ammonium cation-modified cellulose (QACC) nanofiber, electrospun with cellulose acetate (CA) from recycled cigarette filters, into the PEO electrolyte matrix. The nitrogen atom within the quaternary ammonium group exhibits a pronounced affinity for polysulfide compounds, effectively curtailing polysulfide migration. Concurrently, Lewis acid-base interactions between quaternary ammonium groups and lithium salt anions facilitate the release of additional Li+, achieving a lithium-ion transference number 1.5 times higher than its pure PEO counterpart. Furthermore, the introduction of a larger trifluoromethanesulfonimide (TFSI) group on the QACC macromolecule (TFSI-QACC) disrupts the ordered arrangement of PEO macromolecules, resulting in a noteworthy enhancement in ionic conductivity, reaching 2.07 × 10−4 S cm−1 at 60 °C, thus addressing the challenge of low PEO electrolyte conductivity. Moreover, the nanofiber enhances the mechanical strength of the PEO electrolyte from 0.49 to 7.50 MPa, mitigating safety concerns related to lithium dendrites puncturing the electrolyte. Consequently, the composite PEO demonstrates exemplary performance in lithium symmetrical batteries, enduring 500 h of continuous operation and completing 100 cycles at both room and elevated temperatures. This integrated approach, transitioning from waste to wealth, adeptly addresses a spectrum of challenges in the efficiency of solid-state electrolytes, holding considerable promise for advancing lithium‑sulfur battery technology.

Enhanced all-solid-state battery performance through in-situ construction of interface modification layer

The development of high-performance all-solid-state lithium batteries (ASSLBs) relies on improving the interface stability between layered oxide cathodes and sulfide electrolytes, as well as the structural stability of cathode active materials. While coating technology is considered an effective solution, the fabrication of these coating materials using economically viable and scalable manufacturing processes remains a comprehensive and challenging task. In this study, a combination of first-principles calculations and experiments is employed to propose, for the first time, a simple and scalable aqueous process to in-situ construct an Li3VO4 (LVO) buffer coating on the surface of LiCoO2(LCO) cathode, which exhibits high ionic conductivity, relatively low electronic conductivity, and high oxidation limit. The LVO buffering coating not only facilitates the migration of lithium ions at the interface, effectively suppresses interface side reactions, and reduces interface impedance, but also enhances the mechanical and structural stability of the cathode material. As a result, the LCO/LPSC/Li-In ASSLBs with 2% LVO coating exhibit an initial discharge capacity of up to 145.6 mAh g−1 at room temperature (0.1C), with a capacity retention of 94.89% after 100 cycles. Furthermore, the ASSLBs demonstrate good capacity and cycle stability under extreme testing conditions, including high voltage, high temperature, and low temperature, especially exhibiting an initial discharge capacity of up to 114.9 mAh g−1 at −20 °C.

The first-principles study on electrochemical performance, mechanical properties, and lithium-ion migration of LiFePO4 modified by doping with Co and Nb

The first-principles study on electrochemical performance, mechanical properties, and lithium-ion migration of LiFePO4 modified by doping with Co and Nb

Effect of Sr and Nb co-doped on the total conductivity of Li0.5La0.5TiO3 ceramic electrolytes

The solid electrolyte Li0.5La0.5TiO3 is widely used in solid-state batteries due to its high grain conductivity at room temperature (RT). However, the ever-increasing requirement for high ionic conductivity necessitates the improvement of its total conductivity. In this study, tuning the total conductivity of perovskite-type La2/3-xLi3xTiO3 (LLTO) membranes through a co-doping strategy was proposed and systematically investigated, Here, an Li0.5−y+x Sr x La0.5−x Ti1−y Nb y O3 (LLSTN, x = 0, 0.04, 0.06, 0.08, and 0.1 mol%) ceramic solid electrolyte was prepared via the conventional solid-state reaction method. The introduction of Sr2+ and Nb5+ increases the lithium-ion vacancies and transforms the Li0.5La0.5TiO3 crystal structure from tetragonal to cubic. On the other hand, the lattice constant becomes larger, causing the migration channel of the lithium ions to become larger. Meanwhile, with the increase of Nb5+ doping amount, lithium lanthanum niobate forms between grains, inhibiting grain growth and it helps to reduce the resistance of lithium ion migration at grain boundaries. The total conductivity of sample Li0.5La0.42Sr0.08Ti0.92Nb0.08O3 reaches 5.10 × 10−5S·cm−1 at RT, which is about six times higher than that of the undoped sample, and the activation energy is 0.28 eV.

Interface regulation strategy in constructing ZnS@MoS2 heterostructure with enhanced surface reaction dynamics for robust lithium-ion storage

Heterostructure construction is an effective method used to synthesize lithium-ion battery anode materials with high electrochemical performance. In this study, an interface regulated ZnS@MoS2 heterostructure was achieved through a designed solvothermal strategy. The designed strategy introduces interface regulation in the heterostructure, increasing active sites for lithium adsorption and improving the overall dynamics of lithium-ion storage. The build-in electric field is introduced at the interfaces enhancing electron transfer and lithium migration. Ex-situ analyses confirmed the enhanced lithium storage performance in the heterostructure is derived from the stepwise reaction mechanism and the stepwise reactions contribute to cycling stability. DFT calculations revealed electron redistribution at the interfaces in the heterostructure boosting the lithium-ion migration and electron transfer. The interface regulated ZnS@MoS2 heterostructure exhibits outstanding lithium-ion storage performances in both half and full cells. Specifically, the high capacity of 996.0 mAh g−1 is achieved at 5 A g−1 after 1000 rounds, demonstrating remarkable lithium storage performance. This research presents a promising approach to enhance heterostructure electrochemical performance through interface regulation strategies.