Ultrahigh Capacity Research Articles

Cobalt vacancy boosting Co3-xO4@C with superior pseudocapacitive lithium storage

The Co3O4 as anode for lithium ion batteries (LIBs) suffers the sluggish electrode kinetics and severe capacity fade during the cycles. The defective engineering of Co3O4 with oxygen/cobalt defects is an effective strategy to optimize Co3O4 with enhanced electrochemical properties. Herein, a series of 3D inter-connected Co3-xO4@C-y nanostructures with abundant Co defects are synthesized through a hydrothermal approach with subsequent heating-controlled process. Benefiting from its rich surface cobalt-defective sites and the 3D interconnected frameworks, as well as its high surface area and residual carbon layer, the Co3-xO4@C-y synthesized at y = 400 °C as anode for LIBs displays superior pseudocapacitive lithium storage properties with an ultra-high reversible specific capacity of 1900.7 mAh g−1 at 0.2 A g−1, excellent rate capability (e.g., 1415.1 mAh g−1 at 10 A g−1) and ultra-long cycling stability (e.g., 1160.5 mAh g−1 at 15 A g−1 after 2000 cycles).

H+/Cu2+ co-assisted corrosion synthesis of sustainable silicon dendrite anodes

Silicon (Si)-based materials have been identified as next-generation preferred anode materials owing to their ultra-high specific capacity, environmental friendliness and low price. However, the defects in Si-based materials (e.g., the large volume change with unstable solid electrolyte interface during repeated lithiation/delithiation processes and low intrinsic conductivity), will significantly destroy the integrity of electrode structure and get slow dynamic performance, resulting in a fast capacity fading. Herein, we prepared various silicon‑aluminum‑copper dendrites (named SCD-1/2/3) via a two-step displacement dealloying process, which was devoted to simultaneously improving structural instability, low ionic/electronic conductivity of Si crystals. Therefore, the SCD-2 anode possessed an initial Coulombic efficiency of 80 % and exhibited a superior capacity of 1851.7 mA h g−1 at 1 A g−1 after 100 cycles. This paper provides a simple method to gain the Si anodes with high initial Coulombic efficiency, relieved volume expansion and long cycling life.

Preparation of porous composite hydrogel with ultra-high dye adsorption capacity based on biochar: Adsorption behaviors and mechanisms

With the continuous development of industrialization, dyes in industrial wastewater have become a serious environmental issue. To address this environmental issue, a biochar-based composite hydrogel (PAS/aBC-CD) was designed. The use of a simple composite method effectively resolves the challenge of biochar recovery. Furthermore, the modified adsorbent exhibits remarkably high adsorption capacities for all three dyes (MB: 1494 mg/g, MG: 1182 mg/g, and NR: 1031.6 mg/g). It is noteworthy that binary co-adsorption experiments have demonstrated that CrO42− can act as a bridging agent to enhance the adsorption of dyes by the adsorbent. Systematic adsorption–desorption experiments have demonstrated the outstanding recyclability of PAS/aBC-CD, maintaining 98 % of its adsorption capacity after 5 cycles. Additionally, its industrial application potential was demonstrated through column adsorption experiments. In conclusion, this study utilized a simple composite method to produce an adsorbent with high adsorption performance and industrial application potential.

Cation-Loaded Porous Mg2+-Zeolite Layer Direct Dendrite-Free Deposition toward Long-Life Lithium Metal Anodes.

Lithium metal, with ultrahigh theoretical specific capacity, is considered as an ideal anode material for the lithium-ion batteries. However, its practical application is severely plagued by the uncontrolled formation of dendritic Li. Here, a cation-loaded porous Mg2+-Zeolite layer is proposed to enable the dendrite-free deposition on the surface of Li metal anode. The skeleton channels of zeolite provide the low coordinated Li+-solvation groups, leading to the faster desolvation process at the interface. Meanwhile, anions-involved solvation sheath induces a stable, inorganic-rich SEI, contributing to the uniform Li+ flux through the interface. Furthermore, the co-deposition of sustained release Mg2+ realizes a new faster migration pathway, which proactively facilitates the uniform diffusion of Li on the lithium substrate. The synergistic modulation of these kinetic processes facilitates the homogeneous Li plating/stripping behavior. Based on this synergistic mechanism, the high-efficiency deposition with cyclic longevity exceeding 2100h is observed in the symmetric Li/Li cell with Mg2+-Zeolite modified anode at 1mA cm-2. The pouch cell matched with LiFePO4 cathode fulfills a capacity retention of 88.4% after 100 cycles at a severe current density of 1 C charge/discharge. This synergistic protective mechanism can give new guidance for realizing the safe and high-performance Li metal batteries.

Potassium-Hydrogen Hybrid Ion Alkaline Battery: A New Rechargeable Aqueous Battery Combined a K+ Storage Cathode and an Electrochemical Hydrogen Storage Anode.

A rechargeable aqueous hybrid ion alkaline battery, using a proton and a potassium ion as charge carriers for the anode and cathode, respectively, is proposed in this study by using well-developed potassium nickel hexacyanoferrate as the cathode material and mesoporous carbon sheets as the anode material, respectively. The constructed battery operates in a concentrated KOH solution, in which the energy storage mechanism for potassium nickel hexacyanoferrate involves the redox reaction of Fe2+/Fe3+ associated with potassium ion insertion/extraction and the redox reaction of Ni(OH)2/NiOOH. The mechanism for the carbon anode is electrochemical hydrogen storage. The cathode made of potassium nickel hexacyanoferrate exhibits both an ultrahigh capacity of 232.7 mAh g-1 under 100 mA g-1 and a consistent performance of 214 mAh g-1 at 2000 mA g-1 (with a capacity retention of 92.8% after 200 cycles). The mesoporous carbon sheet anode exhibits a capacity of 87.6 mAh·g-1 at 100 mA g-1 with a good rate and cyclic performance. The full cell provides an operational voltage of 1.55 V, a capacity of 93.6 mAh g-1 at 100 mA g-1, and 82.4% capacity retention after 1000 cycles at 2000 mA g-1 along with a low self-discharge rate. The investigation and discussion about the energy storage mechanisms for both electrode materials are also provided.

First-principles prediction of one-dimensional conductive metallic organic polymers as ultrahigh energy density anode for lithium-ion batteries.

Metal-Organic Polymers (MOPs) have attracted growing attention for lithium-ion battery (LIB) applications due to their merits in orderly ionic transportation and robust structure stability in electrochemical reactions. However, they suffer from poor electronic conductivity. In this work, we apply first-principles density functional theory to explore the potential of three one-dimensional (1D) electrically conductive C6H2S4TM (TM = Fe, Co, and Ni) MOPs with the π-d conjugated coordination as anode materials for Li+ ions storage. Our theoretical results reveal that these 1D MOPs possess a superior theoretical capacity of over 748 mA h g-1. In particular, the 1D C6H2S4Ni MOP shows an exceptional theoretical specific capacity of 1110 mA h g-1 based on the three-electron transferring reaction, which significantly outperforms the traditional graphite-based anode material in LIBs. Moreover, the resonant charge transfer between Ni metal and ligand within the 1D C6H2S4Ni MOP reduces the diffusion energy barrier of the Li atoms when they migrate on the surface of the MOP. The ultrahigh theoretical specific capacity of the C6H2S4Ni MOP predicts that it can be a promising anode material for LIBs.

A simple and effective approach to relieve stress and enhance cyclability of Si-based materials toward high-energy lithium-ion batteries

Silicon-based materials are promising anodes to keep up with the demands for next-generation lithium-ion batteries in the coming decades owing to their ultrahigh theoretical capacities. However, the severe volume changes and mechanical fractures during cycling greatly hinder their way to commercialization. So far, it still remains a great challenge to develop advanced Si-based electrodes with high mechanical stability and remarkable electrochemical properties. In this work, we propose a simple and effective strategy to encapsulate Si@SiOx particles into B, N co-doped carbon nanotubes (BNCNTs) to develop Si@SiOx@BNCNT electrode for enhanced lithium storage. The SiOx layer upon Si particle is designed to mitigate the volume expansion of Si and maintain the particle integrity. Finite element analysis demonstrates that BNCNTs with high mechanical strength can further relieve the internal stress induced by Si expansion upon lithiation. The double restraint effect from SiOx layers and BNCNTs on the Si particles contributes to excellent resistance to structural degradation, enabling high stability and desirable electrochemical performance of Si@SiOx@BNCNT electrode. This strategy provides great opportunities for the practical application of Si-based anodes in high-energy lithium-ion batteries.

Metal-organic frameworks based on ternary transition metal ions for high-performance lithium ion batteries

Metal-organic frameworks (MOFs) materials have been widely researched in energy conversion systems because of porosity and active sites. However, applying MOF as an electrode material remains challenging because of its structural instability. In this work, two novel materials are designed to promote the research of MOFs-based electrode materials for lithium-ion batteries (LIBs). Two ternary metallic ions (Mn2+, Co2+, Ni2+) constituent MOFs with two- and three-dimensional (3D) structures are synthesized by combining with benzene-1,2,3,4,5,6-hexacarboxylate (BHC) ligand via a simple hydrothermal method. The structures of MCN-1 and MCN-2 belong to monoclinic symmetry, C2/c space group. The 3D structure of MCN-2 can enhance the interfacial contact between electrode materials and electrolytes and provide more active sites for the storage of Li+. Electrochemical experiments show that the 3D structure ternary MOF delivers an ultra-high capacity of 807.3 mAh g−1 after 100 cycles at 100 mA g−1, even though a phase transition occurs during the electrochemical process. This superior performance is rationally owing to the synergetic mechanism of intercalation/deintercalation combined with capacitance behavior, which has broad application prospects as anode material.

Nickel aerogel @ ultra-thin NiCo-LDH nanosheets integrated freestanding film as a collaborative adsorption and accelerated conversion cathode to improve the rate performance of lithium sulfur batteries

It is a great challenge to develop freestanding ultralight cathodes for lithium–sulfur battery exhibiting good electrochemical performances. Herein, ultrathin porous nickel–cobalt layered double hydroxide (NiCo-LDH) nanosheets were grown on the surface of ultra-light nickel microwire aerogels (NMWAs), and there is capillary action in the gaps formed by the ordered arrangement due to the presence of magnetic filed in the preparation process, which has the advantages of synergistic adsorption and accelerated conversion kinetics of lithium polysulfide. Because of the abundant hydrophilic hydroxyl groups on the surface of NiCo-LDH and the capillary action of NMWAs, the integrated freestanding film cathode sulfur host (NMWAs@NiCo-LDH/S) provides excellent rate performance as well as cycling stability. The film cathode has an ultra-high initial specific capacity of 1238.4 mAh g−1 at 0.1C and an excellent reversible capacity of 805.8 mAh/g at 5.0C. Even after 700 cycles at a high current density of 5.0C, it still provides a reversible capacity of 647.1 mAh g−1 with a capacity decay rate of only 0.018 % per cycle. This work provides a simple and new way for the design of high rate lithium–sulfur battery film cathodes with good cycle stability.

Engineering of lithiophilic hosts for stable lithium metal anodes

Lithium (Li0) metal has been deemed the desired anode for the future of cutting-edge rechargeable Li batteries benefiting from its lowest reduction potential and ultrahigh theoretical specific capacity. Nevertheless, the large-scale applications of Li metal batteries are restricted by scattered Li dendrite formation and uncontrollable volume expansion. To address these issues, a currently prevalent measure is to use structured lithiophilic hosts for Li metal. The enhanced lithiophilicity of hosts is significant for regulating the Li nucleation barrier. By virtue of these lithiophilic measures, the Li nucleation sites will be well controlled and the Li plating layer will be more stable. Through this article, we classified various lithiophilic hosts and described their applications for Li metal batteries, including heteroatom-doping carbon, lithiophilic-material loading hosts and gradient skeletons. We discussed the inherent advantages and lithophilic mechanisms of these hosts on optimizing the lithophilic properties and analyzed various factors that induced the formation of dendrite Li. Moreover, the review outlines the current challenges and perspectives for Li metal anodes, and some understanding of the lithiophilic chemistry is given.

Ultrahigh and kinetic-favorable adsorption for recycling urea using corncob-derived porous biochar

Insufficient attention has been given to the recycling of excess urea despite its potential detrimental effects on soil nutrient equilibrium, geological structure, and crop health. In this study, corncob-derived porous biochar (CPB), which is rich in surface functional groups, was prepared from biomass corncob in two steps as an adsorbent to remove urea from wastewater. Compared with the typical carbonization and activation processes, this process resulted in a higher yield of CPB and an ultrahigh adsorption capacity for urea. Response surface analysis was utilized to determine the optimal carbonization conditions, which were found to be 500 °C for 6 h with a heating rate of 15 °C/min. The exceptional adsorption capability of CPB can be ascribed to its porous structure and significant presence of oxygen-containing functional groups, which facilitate a synergistic interaction of physisorption and chemisorption. This adsorption phenomenon aligns with the Harkins–Jura isotherm model and adheres to pseudo-second order kinetics. CPB demonstrates potential as an adsorbent for the elimination of urea from wastewater in an economical and effective fashion.

Accelerating lithium-sulfur battery reaction kinetics and inducing 3D deposition of Li2S using interactions between Fe3Se4 and lithium polysulfides

Although lithium-sulfur batteries (LSBs) exhibit high theoretical energy density, their practical application is hindered by poor conductivity of the sulfur cathode, the shuttle effect, and the irreversible deposition of Li2S. To address these issues, a novel composite, using electrospinning technology, consisting of Fe3Se4 and porous nitrogen-doped carbon nanofibers was designed for the interlayer of LSBs. The porous carbon nanofiber structure facilitates the transport of ions and electrons, while the Fe3Se4 material adsorbs lithium polysulfides (LiPSs) and accelerates its catalytic conversion process. Furthermore, the Fe3Se4 material interacts with soluble LiPSs to generate a new polysulfide intermediate, LixFeSy complex, which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of Li2S, enhancing the reversibility of LSBs. The designed LSB demonstrates a high specific capacity of 1529.6 mA h g−1 in the first cycle at 0.2 C. The rate performance is also excellent, maintaining an ultra-high specific capacity of 779.7 mA h g−1 at a high rate of 8 C. This investigation explores the mechanism of the interaction between the interlayer and LiPSs, and provides a new strategy to regulate the reaction kinetics and Li2S deposition in LSBs.

Accelerated Sulfur Redox Kinetics on Transition Metal Sulfide Electrocatalysts by Modulating Electronic‐State of Active Sites

AbstractLithium‐sulfur (Li‐S) batteries are considered a competitive next‐generation electrochemical energy storage device, while the shuttle effect of soluble lithium polysulfides (LiPSs) resulting from the sluggish redox kinetics severely impedes their practical applications. Herein, a novel cation doping strategy is demonstrated for substantially accelerating the sulfur redox kinetics on the transition metal sulfide (TMS) electrocatalysts by partially substituting cobalt atoms with in situ dissolved Ni dopants (NixCo3‐xS4, 0<x≤1). Theoretical calculations revealed that the doping of Ni in the spinel Co3S4 phase enables the electronic‐state modulation of metal active sites by realizing the upshift of the d‐orbital center, thus leading to good chemical adsorption of intermediates and low redox conversion barriers between LiPSs and solid Li2S products. This is confirmed by in‐depth electrochemical dynamics and in situ Raman characterizations, in which the obtained Ni0.5Co2.5S4 with hierarchical nanosheet structure delivers the stronger chemical affinity of Li2S6 and higher precipitation/dissociation capacity of Li2S in comparison to monometallic cobalt sulfides. Benefiting from these outstanding attributes, the assembled Li‐S batteries by incorporating Ni0.5Co2.5S4 electrocatalysts into S@carbon nanotube cathode (S@Ni0.5Co2.5S4/CNT) exhibit a high specific capacity of 1189 mAh g−1 with excellent rate performance of 596 mAh g−1 at 5 C and long‐term cycling performance over 600 cycles with a capacity decay of 0.06% per cycle at 1 C. More importantly, an ultrahigh reversible areal capacity of 6.6 mAh cm−2 can be achieved for S@Ni0.5Co2.5S4/CNT cathode even with a high sulfur loading of 6.1 mg cm−2. This work demonstrates a new insight into designing TMS electrocatalysts toward rapid redox conversion kinetics in Li‐S batteries.

Boosting the ORR/OER Activity of Cobalt-Based Nano-Catalysts by Co 3d Orbital Regulation.

The transition metal oxides/sulfides are considered promising catalysts due to their abundant resources, facile synthesis, and reasonable electrocatalytic activity. Herein, a significantly improved intrinsic catalytic activity is achieved for constructing a Co-based nanocrystal (Co-S@NC) with the coordination of Co─S, Co─S─C, and Co─Nx─C. The calculational and experimental results demonstrate that the diversified chemical environment of Co-cations induces the transition of 3d orbitals to a high spin-state that exhibits the coexistence of Co2+ with fully occupied dπ orbitals and Co3+ with unpaired electrons in dπ orbitals. The diverse dπ orbitals occupation contributes to an elevated d-band center of Co ions, which accelerates oxygen reduction reaction and oxygen evolution reaction electrocatalytic kinetics of the Co-S@NC nanocrystal. Therefore, the Li-O2 batteries with Co-S@NC as cathode catalyst exhibit 300 cycles at the current density of 500 mA g-1 with a cut-off capacity of 1000 mAh g-1. Moreover, the ultrahigh discharge specific capacity of 34 587 mAh g-1 is obtained at a current density of 1000 mA g-1, corresponding to the energy density 949 Wh kg-1 of a prototype Li-O2 battery. The study on 3d orbital regulation of nanocrystals provides an innovative strategy for bifunctional electrocatalysts toward the practical application of metal-air batteries.

Achieving a smooth “adsorption-diffusion-conversion” of polysulfides enabled by MnO2-ZnS p-n heterojunction for Li-S battery

The commercial application of lithium-sulfur batteries is primarily impeded by the constant shuttling of soluble polysulfides and sluggish redox kinetics. Nowadays, the discovery of the heterojunction, which combines materials with diverse properties, offers a new perspective for overcoming these obstacles. Herein, a functional coating separator for the lithium-sulfur battery is designed using a MnO2-ZnS p-n heterojunction with a spontaneous built-in electric field (BIEF). The MnO2 nanowire provides suitable adsorption capacity for polysulfides, while the abundant reactive sites brought by ZnS ensure efficient conversion. Moreover, the BIEF significantly facilitates the migration of electrons and polysulfides at the MnO2-ZnS interface, enabling a smooth “adsorption-diffusion-conversion” reaction mechanism. By serving as both the adsorption module and catalytic sites, this BIEF allows batteries utilizing separators modified with MnO2-ZnS heterojunction to achieve an impressive initial capacity of 1511.1 mAh g−1 at 0.1C and maintain a capacity decay rate of merely 0.048% per cycle at 2.0C after 1000 cycles. Even when increasing sulfur loading to 9.4 mg cm−2 in lean electrolyte (5.4 μL mg−1), the battery still exhibits an ultrahigh areal capacity of 6.0 mAh cm−2 after 100 cycles.

Dual-selective silver recovery strategy by simultaneous adsorption-reduction boosted by in-situ magnetic field

The mainstream silver recovery has problems such as resource waste, weak silver selectivity, and complicated operation. Here, self-propelled magnetic enhanced capture hydrogel (magnetic NbFeB/MXene/GO, MNMGH) was prepared by self-crosslinking encapsulation method. MNMGH achieved high selectivity (Kd = 23.31 mL/g) in the acidic range, and exhibited ultrahigh silver recovery capacity (1604.8 mg/g), which greatly improved by 66% with the assistance of in-situ magnetic field. The recovered silver crystals could be directly physically exfoliated, without acid/base additions. The selective sieving effect of adsorption, MNMGH preferentially adsorbed Ag(I), and then selectively reduced to Ag(0), realizing dual-selective recovery. The in-situ magnetic field enhanced selective adsorption by enhancing mass transfer, reactivity of oxygen-containing functional groups. Furthermore, density function theory simulations demonstrated that the in-situ magnetic field could lower the silver reduction reaction energy barrier to enhance the selective reduction. Three-drive synergy system (reduction drive, adsorption drive and magnetic drive) achieved ultrahigh silver recovery performance. This study pioneered an in-situ magnetic field assisted enhancement strategy for dual-selective (adsorption/reduction) recovery of precious metal silver, which provided new idea for low-carbon recovery of noble metal from industrial waste liquids.

HsGDY 3D Framework-Encapsulated Cu2O Quantum Dots for High-Efficiency Energy Storage.

Nanostructured electrode materials become a vital component for future electrode materials because of their short electron and ion transport distances for fast charge and discharge processes and sufficient space between particles for volume expansion. So, achieving a smaller size of the nanomaterial with stable structure and high electrode performance is always the pursuit. Herein, the hybrid electrode material system hydrogen-substituted graphdiyne (HsGDY)/Cu2O-quantum dots (QDs) composed of an active carbon substrate and vibrant metal oxide QD load was established by HsGDY and cuprous oxide. The HsGDY frame with conjugated structure not only delivers impressive capacity by a self-exchange mechanism but also characterizes a matrix to forge strong connections with numerous active Cu2O-QDs for the prevention of aggregation, leading to a homogeneous storage and transport of charge in a bulk material of crisscross structural pores. QD-based electrode materials would exhibit desired capacities by their large surface area, abundant active surface atoms, and the short diffusion pathway. The hybrid system of HsGDY/Cu2O-QDs delivers an ultrahigh capacity of 1230 mA h g-1 with loading density reaching up to 1 mg cm-2. In the meantime, the electrode exhibits a long cycle stability of over 8000 cycles. The synergistic effect endows the hybrid system electrode with an approximately theoretical energy density, suggesting the great potential of such carbon/QD hybrid material system applied for high-performance batteries.

Additives strategies to improving cycling stability of Li metal batteries by modifying electrode electrolyte interphases

Li metal batteries (LMBs) have attracted much attention due to the ultra-high theoretical capacity of the Li metal anode (LMA). However, the uncontrollable dendrites growth and low coulombic efficiency hinder their practical application. Here, we explore 3,5-difluoropyridine (2F-BD) as a novel electrolyte additive to enable high-performance LMBs. The 2F-BD additive participates in and modifies the solvation structure of Li ions by reducing the coordinated number of PF6− at the electrode surface, leading to the formation of a LiF and Li3N-rich solid electrolyte interphase (SEI). The LiF component increases the robustness of SEI and suppresses the formation of Li dendrites, while the Li3N component facilitates the transportation and reaction kinetics of Li ions. As a result, the Li||Li symmetric cell presents a stable cycling performance of up to 500 ​h at a current density of 1 ​mA ​cm−2. After coupling with LiFePO4 cathode, the obtained full cell achieves high specific capacities of 106.06 ​mA ​h ​g−1 and 84.98 ​mA ​h ​g−1 at 2.55 ​mA ​cm−2 and 5.10 ​mA ​cm−2, respectively, and maintains a high capacity retention of 84.0% after 1000 cycles at 0.13 ​mA ​cm−2, with an average cycling CE of 99.58%.

Insight of the evolution of structure and energy storage mechanism of (FeCoNiCrMn)3O4 spinel high entropy oxide in life-cycle span as lithium-ion battery anode

Recently, spinel high-entropy oxide (HEO) anode materials have garnered extensive attention for high-energy lithium-ion batteries due to their high specific capacity. Many studies have explored its energy storage mechanism, but few have paid attention to its characteristics in long cycle life. In this work, the whole life cycling performance of (FeCoNiCrMn)-HEO is presented and investigated for the first time. Distinct capacity trends are studied to divide the cycling life into three stages: activation, upgradation, and degradation. Ex situ morphological characterizations are conducted to reveal that the driving force of stage change is continuous particle fragmentation. As a result, refined particles promote conversion reaction reversibility and induce extra interfacial capacity, achieving 2831 mAh g−1 at 825 cycles. Density functional theory (DFT) calculations provide a deeper insight into the high entropy effect on the ultra-high extra interfacial capacity. However, continuous refinement brings about huge electrolyte interface-derived layers, which are also responsible for pre-decay and post-collapse. The view of the evolution of the lithium storage mechanism is explicitly presented and experimentally verified by high-energy ball milling and fluorinated vinyl carbonate (FEC). These above results can give practical solutions to design high specific capacity and long-life cycle stability HEO anode in the future.

Electron-repulsion effect of anti-solvent strategy for long-cycle nickel sulfide-containing potassium-ion batteries

Transition metal dichalcogenides experience severe structural degradation when used as anodes in potassium-ion batteries, resulting in undesirable electrochemical behaviors. To tackle this challenge, a novel approach involving "anti-solvent-enhanced local high-concentration electrolytes" was proposed to enhance the electrochemical stability of transition metal dichalcogenides for potassium-ion storage. This improvement is attributed to the facilitation of the aggregation of local solvation structures within the ether-based electrolyte. We demonstrate the effectiveness of this method by utilizing nickel sulfide composite materials. By diluting the ether-based high-concentration electrolyte with 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (HFE) anti-solvent, the nickel sulfide containing anode achieved an ultra-high specific capacity of 382 mAh g−1 after 1500 cycles at 1 A g−1. We found that the HFE anti-solvent, with its high concentration of negatively charged fluorine atoms, exerts a strong electron-repulsion effect on the bis(fluorosulfonyl)imide anions, promoting the aggregation of local solvation structures. It not only lowers the desolvation energy but also exhibits high stability during interactions with the interface, thereby improving and keeping the K-ion’s migration ability. This, in turn, improves the cycling stability of the electrode during the potassiation-depotassiation process. We believe that this new strategy of improving potassium-ion storage performance will drive advancements in related fields.