Application Of Lithium-sulfur Batteries Research Articles

Favorable Moderate Adsorption of Polysulfide on FeNi3 Intermetallic Compound Accelerating Conversion Kinetics for Advanced Lithium-Sulfur Batteries.

Sluggish conversion kinetics of polysulfides during discharge and the severe shuttle effect significantly hinder the practical application of lithium-sulfur (Li-S) batteries. In this work, the lattice engineering strategy of Fe hybridization is employed to manipulate the bulk phase spacing of FeNi3 (space group Pm3m) intermetallic compounds to adjust the 3d electronic structure, optimizing the adsorption of polysulfides, thereby accelerating the catalytic conversion. As a result, FeNi2.25@OC achieves favorable moderate adsorption toward polysulfides. Due to the larger number of electrons occupying the lowest occupied molecular orbital of Li2S4, the S-S bonds are weakened and broken. Temperature-dependent experiments confirm that FeNi2.25@OC exhibits the lowest activation energy and can effectively accelerate the catalytic conversion of polysulfides. The Li-S cell assembled with FeNi2.25@OC modified PP separator delivers a high initial discharge specific capacity of 1219.5 mAh g-1 at 0.2 C. Even at a high sulfur loading of 6.06mg cm-2 and lean electrolyte conditions (6 µL mg-1), it can cycle stably for 60 cycles.

Replenish the Electron-Deficient State of Carbonyl Carbon Atoms to Achieve Stable Li-S Battery.

Carbonate-based electrolytes are widely used in Li-ion batteries (LIBs) due to their safe, stable properties and wide operating temperature range. However, the nucleophilic attack at carbonyl carbon atoms by polysulfide anions and the low solubility of lithium nitrate (LiNO3<0.1m) in carbonate-based electrolytes seriously hinder the application of lithium-sulfur (Li-S) batteries in carbonate-based electrolytes. Herein, the electrophilicity of carbonyl carbon atoms is gradually reduced through solvent molecules redesign, eliminated the attack of polysulfide anions on carbonyl carbon atoms, and also changed the intermolecular interactions in the electrolyte, improving the solubility of LiNO3 (>1.0m) and forming stable LiNxOy-containing SEI on the surface of the lithium metal. The assembled Li-S battery with these designed solvent molecules delivers an initial discharge capacity of 1251.7mAhg-1 at 0.1C. In addition, the lithium-sulfur battery assembled with the designed solvent molecule has a discharge capacity of 631mAhg-1 after 420 cycles at 0.2 C, with a capacity retention of ≈60%. Moreover, the Li||Li symmetrical cell shows stable cycle performance over 1200h at 0.5mAcm-2 and 0.5mAhcm-2.

Interface engineering of heterostructural quantum dots towards high-rate and long-life lithium-sulfur full batteries

Despite being as next-generation energy storage systems with ultra-high theoretical energy density of 2600 Wh kg−1, lithium-sulfur (Li-S) batteries face serious hurdles due to the sluggish redox kinetics in S cathodes and uncontrollable growth of dendrites in Li anodes. To simultaneously address such issues, herein, we present an interface engineering strategy to develop a dual-functional host for S cathode and Li anode, which is constructed by heterostructural WC-WN0.67 quantum dots homogeneously embedded in N-doped graphene nanosheets (WC-WN0.67@NG). As a result, the Li-S full batteries deliver a high reversible capacity of 704 mA h g−1 even at a high rate of 4 C, and demonstrate a long-term cycling stability even at 2 C with a low degradation rate of 0.027 % over 1200 cycles. This work paves the way to facilitate the practical applications of Li-S batteries through interface engineering of dual-functional heterostructural quantum-dot host.

A polysulfides adsorption strategy through cation-anion interactions for achieving high-safety lithium-sulfur batteries in multiple scenarios

The widespread application of lithium-sulfur batteries (LSBs) is hindered by challenges such as the shuttle effect of polysulfides (LiPSs), slow reaction kinetics, and fire safety concerns. In this study, surface-functionalized boron nitride nanosheets (ChBN) are prepared and employed as functional separator coatings, enabling multiple application scenarios of LSBs. Specifically, a creative strategy of cation-anion interactions is constructed through the strong chemisorption of N+ on the ChBN surface to Sn- in LiPSs. In addition, the boron nitride and N+ show synergistic effects on adsorption-catalysis, further facilitating the rapid and sufficient deposition of Li2S. The prepared LSBs with ChBN + SP/PP separators exhibit excellent cycle stability (an ultralow capacity degradation of 0.034 % per cycle over 500 cycles at 2C). These LSBs are available in a wide temperature range of −20 to 60 °C, offering a capacity of 1208 mA h/g at 60 °C and 919 mA h/g at −20 °C. Furthermore, the presence of ChBN effectively improves the fire-safety of pouch batteries through the condensed-phase flame retardant mechanism. This simple fabrication process of ChBN is effective and favorable for large-scale manufacturing, which provides a feasible method for the development of high-safety LSBs.

Spatial structure design of interlayer for advanced lithium–sulfur batteries

The practical application of lithium-sulfur (Li–S) batteries has been hindered by the lithium polysulfide shuttle effect. An effective way to solve this problem is to utilize interlayer engineering to confine polysulfides and promote their catalytic conversion. From a spatial perspective, we designed a carbon nanofiber conductive layer (CNF, without Sn content, labeled as 0) and two Sn-doped carbon nanofiber catalytic layers (SCNF, with 10 wt% and 20 wt% Sn content, labeled as 1 and 2, respectively) with different contents of catalyst content, and verified an efficient interlayer structure by adjusting the order of preferential contact between the conductive layer and the catalytic layer with the sulfur cathode to form a hierarchical system for the inhibition and conversion of lithium polysulfide. Electrochemical measurements show that different spatial configurations have significant discrepancies on the electrochemical performance of Li–S batteries. Thus, the space configuration of 210 enables the Li–S battery to provide a specific capacity of up to 1088 mAh g−1 after 100 cycles at 0.2C. Even under the harsh conditions of high sulfur loading (5.6 mg cm−2) and lean electrolyte (E/S = 10 μL mg−1), the Li–S battery was able to cycle stably for 94 cycles at 0.2C with 87 % capacity retention. This study provides a novel spatial strategy for advancing the spatial design of high-performance Li–S batteries.

Synergistic implementation of efficient adsorption-diffusion-conversion in lithium-sulfur batteries via built-in electric field constructed by transition metal selenides

The adsorption of lithium polysulfides (LiPSs), the transport of lithium ions, and the redox kinetics collectively play pivotal roles in determining the application of lithium-sulfur (Li-S) batteries. Herein, a defect-rich p-Co3Se4/n-ZnSe p-n junction (ZCSNC) is engineered by chemical vapor deposition (CVD)-selenation. The n-type semiconductor ZnSe and the p-type semiconductor Co3Se4 contained in ZCSNC effectively anchor LiPSs and promote the catalytic reaction kinetics through synergistic effects, respectively. Meanwhile, the presence of heterogeneous interfaces in the p-n junction and the difference in work functions spontaneously form a built-in electric field, which promotes the transport and transfer of lithium ions and LiPSs. Therefore, the ZCSNC functional material contributes to improving the electrochemical performance of Li-S batteries through the process of adsorption-diffusion-conversion. The Li-S cells with ZCSNC-modified separators show excellent rate performance (741.1 mAh/g at 5C) and long-lasting cycling performance (only 0.04 % capacity decay per cycle over 1000 cycles). Notably, the ZCSNC still has excellent rate discharge capacities (683.9 and 649.7 mAh/g at 2C, respectively) at high sulfur loading and low temperature of 0 °C. This study illustrates that a p-n junction containing a built-in electric field can effectively modulate the kinetics of redox reactions of LiPSs through synergistic interactions.

Ionic Liquid-Assisted Synthesis of Higher Loaded Ni/Fe Dual-Atom Catalysts in N, F, B Codoped Carbon Matrix for Accelerated Sulfur Reduction Reaction.

In response to mitigating the severe shuttle effect within lithium-sulfur batteries, single-atom catalysts have emerged as one of the most effective solutions. Here, N, F, B codoped porous hollow carbon nanocages (NFB-NiFe@NC) with high Ni and Fe doping are rationally designed and synthesized using ionic liquids (ILs) as dopants. The introduction of ILs inhibits the growth of zeolitic imidazolate framework-8 (ZIF8), resulting in NFB-ZIF8 precursors with smaller particle sizes, enabling higher loading dual-atom catalysts. Meanwhile, the abundant heteroatoms increase the reactive sites and alter the carbon matrix's nonpolar intrinsic properties, thus enhancing the chemisorption of polysulfides. The synergistic interaction of the heteroatoms with Ni and Fe dual-atoms ultimately promotes the catalytic conversion kinetics of polysulfides. As a result of these beneficial properties, the cells prepared using the NFB-NiFe@NC modified separator exhibit significantly improved performance, including a high initial capacity of 1448 mAh g-1 at 0.2 C. Even at a high S-loading of 7.6 mg cm-2, the ideal area capacity of 8.38 mAh cm-2 can still be maintained at 0.1 C. New insights are provided here for designing highly loaded dual-atom catalysts for application in lithium-sulfur batteries.

Ultrafine Mo2N Quantum Dots Embedded in N-Doped Graphene Sheets Enable Efficient Adsorption-Catalytic Transformation of Polysulfides.

Because of the high theoretical energy density of 2600 Wh kg-1, lithium-sulfur batteries (LSBs) are anticipated to be among the next generation of high-energy-density storage technologies. However, the practical application of LSBs has been severely hampered by the significant shuttle effect and slow redox kinetics of polysulfides (LiPSs). To address the above problems, in this paper, the concept of quantum dots (QDs) was introduced to design and synthesize Mo2N QD-modified N-doped graphene nanosheets (marked as Mo2N-QDs@NG), which were used as separator modification materials for LSBs. The experimental results demonstrated that the introduction of Mo2N QDs avoids stacking of graphene sheets and provides more active sites for the conversion of LiPSs. Moreover, Mo2N enhances the chemical fixation and catalyzes the liquid-solid conversion of soluble LiPSs by forming Mo-S and Li-N bonds with LiPSs. Additionally, establishing Mo-C bonds with Mo2N, N-doped graphene sheets can facilitate the transport of electrons and ions and physically prevent the diffusion of LiPSs, thus creating a highly conducting carbon structure to support electrochemical reactions. Benefiting from the synergistic effect of chemical immobilization and catalysis of Mo2N QDs with the physical confinement of NG, Mo2N-QDs@NG-PP batteries exhibit enhanced electrochemical performance.

Synergistic promotion of reaction kinetics for LiPSs at high loadings by interfacial built-in electric field and sulfur vacancies of ternary heterostructure for high-performance Li-S batteries

The practical application of lithium-sulfur batteries is significantly impeded by the chaotic migration of lithium polysulfides, sluggish redox-reaction kinetics, and pronounced shuttle effect. Herein, a ternary heterostructure (MoS2-x/MoO2/CoP) is developed with a spontaneous built-in electric field (BIEF) and enriched sulfur vacancies. This heterostructure comprises MoS2-x, which has a high adsorption capability and work function; CoP, noted for its low work function and potent catalytic properties; and MoO2, which features a work function between that of MoS2-x and CoP and serves as a bridge with excellent electronic conductivity. An appropriate combination of the catalyst and adsorbent with sulfur vacancies controls the direction of the BIEF, realizing the “adsorption-directed migration-catalytic” reaction mechanism for sulfur species. Specifically, the synergetic effect of the BIEF and sulfur vacancies enhances electron migration from CoP to MoS2-x, which improves the lithium polysulfide (LiPSs) trapping and accelerates the directional migration of LiPSs to CoP, thereby enabling the efficient catalytic conversion of sulfur species. Consequently, batteries equipped with MoS2-x/MoO2/CoP interlayers that contain sulfur vacancies demonstrate an ultrahigh initial specific capacity of 1356.2 mA h g−1 at 0.2 C, maintaining a capacity of 708.3 mAh g−1 after 1000 cycles at 2 C. Even with sulfur loading increased to 7.13 mg cm−2, these batteries display an initial specific capacity of 7.2 mAh cm−2. This work provides a feasible approach for the rational design of vacancy-containing ternary heterostructure catalysts for commercial lithium-sulfur batteries.

Separator modification with a high-entropy hydroxyphosphate, Co0.29Ni0.15Fe0.33Cu0.16Ca3.9(PO4)3(OH), for high-performance Li-S batteries

The shuttle effect of lithium polysulfides (LiPSs) significantly hinders the practical application of lithium-sulfur batteries (LSBs). Herein, a high-entropy hydroxyphosphate (Co0.29Ni0.15Fe0.33Cu0.16Ca3.9(PO4)3(OH), denoted as HE-CHP), was synthesized by metal cation exchange with calcium hydroxyphosphate (CHP) and then coated on polypropylene (PP) separators to suppress the shuttling of LiPSs. Density functional theory calculations indicated that the various introduced metal cations could effectively modulate the binding strength of soluble polysulfides and enhance the reaction kinetics of LiPSs conversion. As a result, LSBs using the HE-CHP@PP separator exhibited an excellent discharge capacity (1297 mAh g−1 under 0.2 C) and a slow capacity decay during long-term cycling (0.046 % per cycle at 2 C). At a sulfur loading of up to 6.5 mg cm−2, the LSB with HE-CHP@PP separator displayed a discharge capacity of 5.8 mAh cm−2. Notably, the CNT@S||Li Li-S pouch cell with HE-CHP modified separator delivered an initial energy density of 432 Wh kg−1.

Entrapment and Reactivation of Polysulfides in Conductive Amphiphilic Covalent Organic Frameworks Enabling Superior Capacity and Stability of Lithium-Sulfur Batteries.

Inhibiting the shuttle of polysulfides is of great significance for promoting the practical application of lithium-sulfur batteries (LSBs). Here, an imine-linked covalent organic framework@carbon nanotube (COF@CNT) interlayer composed of triazine and boroxine rings is constructed between the sulfur cathode and the separator for polysulfides reception and reutilization. The introduction of CNT imparts the conductor characteristic to the interlayer attributed to electron tunneling in thin COF shell, and creates a hierarchical porous architecture for accommodating polysulfides. The uniform distribution of amphiphilic adsorption sites in COF microporous structure not only enables efficient entrapment of polysulfides while allowing the penetration of Li+ ions, but also provides a stable electrocatalytic channel for bidirectional conversion of active sulfur to achieve the substantially improved capacity and stability. The interlayer-incorporated LSBs deliver an ultrahigh capacity of 1446mAg-1 at 0.1C and an ultralow capacity decay rate of 0.019% at 1C over 1500 cycles. Even at an electrolyte/sulfur ratio of 6µLmg-1, an outstanding capacity of 995mAhg-1 and capacity retention of 74.1% over 200 cycles at 0.2C are obtained. This work offers a compelling polysulfides entrapment and reactivation strategy for stimulating the study on ultra-stable LSBs.

Polymorph interface strategy presents avenues for kinetics-enhanced and dendrite-free lithium sulfur batteries

Shuttle effect and slow kinetic property are the challenges for the practical application of lithium-sulfur (Li-S) batteries. As an effective strategy, the polymorph effect is applied to rationally design multifunctional catalysts. Herein, the unique polymorph interface was constructed by different CoSe2 crystalline phases, and the systematic investigation on the sulfur cathodes and lithium anode is reported. Carbon nanofiber (CNF) derived from bacterial cellulose (BC) is used as a scaffold for disperse CoSe2 catalysts to construct electrically conductive highways. According to the experimental and calculation results, orthorhombic CoSe2 exhibits superior adsorption capacity and catalytic activity towards LiPSs, while cubic CoSe2 shows better electronic conductivity. Mixed phase CoSe2 not only balances the advantages of both, but also showcases impressive performance due to its unique polymorph interface structure. Besides, uniform lithium deposition can be also achieved. Consequently, the modified separators endow Li-S batteries with a high reversible discharge capacity (700 cycles at 1 C with only 0.063 % capacity decay per cycle) and excellent rate performance (702 mAh g−1 is maintained at 5 C). The pouch cell with separator modifications on both sides was assembled and exhibits a high discharge capacity. This work provides a polymorph interface strategy for the rational design of catalysts.

A bifunctional thiobenzamide additive for improvement of cathode kinetics and anode stability in lithium-sulfur batteries

Lithium-sulfur batteries (LSBs) are considered as the key candidates for the next generation of energy storage devices. However, the practical applications of LSBs are hindered by the slow conversion of sulfur species and the inhomogeneous Li+ precipitation /stripping of lithium anode. Here, we report a bifunctional thiobenzamide electrolyte additive, 4-(trifluoromethyl) thiobenzamide (TFBCA), which synergistically improves cathode redox kinetics and anode stability. Polysulfides (LiPSn) are in-situ transferred to more reactive polysulfide intermediates (T-Sn-T), which significantly improve the liquid–solid reduction process by promoting the deposition dimension of Li2S. A LiF/Li3N-rich solid electrolyte interphase is formed with TFBCA, the uniform lithium deposition is achieved and the growth of lithium dendrites is suppressed. Correspondingly, LSBs with TFBCA show a high capacity (888 mAh·g−1 at 5C) and cycling stability (0.055 % per cycle after 600 cycles at 2C). Even under high sulfur loading (7.1 mg·cm−2) and low E/S ratio of 7, the LSBs also exhibit an areal capacity of 7 mAh·cm−2 after 50 cycles, and an energy density of 314 Wh·kg−1 is achieved for the pouch cell. This work demonstrates an efficient additive strategy through molecular structure design to construct high-performance LSBs.

Ultrathin 2D-2D MXene-LDH Interlayer with High Polysulfide Adsorption Ability for Advanced Li-S Batteries.

Lithium-sulfur (Li-S) batteries are considered as promising energy storage systems due to the high energy density of 2600 W h kg-1. However, the practical application of Li-S batteries is hindered by the inadequate conductivity of sulfur and Li2S, as well as the shuttle effect caused by polysulfides during the charge-discharge process. Introducing a conductive interlayer between the cathode and the separator to physically resist polysulfides represents an effective and straightforward approach to mitigate the shuttle effect in Li-S batteries. In this paper, an ultrathin (<1 μm) 2D-2D MXene-LDH interlayer with high polysulfide adsorption ability was introduced to Li-S batteries. The synergistic effect between MXene and layered double hydroxide greatly improved the adsorption effect of the interlayers: the conductive Ti3C2Tx MXene chemically adsorbs polysulfides and promotes their fast transfer, and the NiCo-LDH alleviates the restack of MXene and facilitates Li+ diffusion. After inserting the MXene-LDH interlayer, the Li-S batteries exhibit an enhanced specific capacity of 1137.6 mA h g-1 at 0.1 C and retain 622.6 mA h g-1 after 100 cycles. The ultrathin 2D-2D interlayer offers a feasible way for the development of highly efficient and lightweight interlayers in Li-S batteries.

A Review of Electrospun Carbon-Based Nanofibers Materials used in Lithium-Sulfur Batteries.

Commercial lithium-ion batteries are gradually approaching their theoretical specific energy, which cannot meet the fast-growing energy storage demands. Lithium-sulfur (Li-S) batteries are anticipated to supersede lithium-ion batteries as the next-generation energy storage system owing to their high atheoretical specific capacity (1675 mAh g-1) and energy density (2600 Wh kg-1). Nonetheless, Li-S batteries encounter several challenges, including the inadequate conductivity of sulfur and lithium sulfide, sulfur's volume expansion, and the shuttle effect of lithium polysulfides, all of which significantly impact the practical utilization of Li-S batteries. Electrospun carbon-based nanofibers can simultaneously resolve these issues with their economical preparation, distinctive nanostructure, and exceptional flexibility. This review presents the most recent research findings on electrospun carbon-based nanofibers materials serving as sulfur hosts and interlayer components in Li-S batteries. We analyzed the impact of the material's structural design on the performance of Li-S batteries and the relative underlying mechanism. Finally, the current challenges and issues faced by carbon-based nanofibers composites in the application of Li-S batteries are summarized, and the future development trajectory are outlined.

N-Vacancy Enriched Porous BN Fibers for Enhanced Polysulfides Adsorption and Conversion in High-Performance Lithium-Sulfur Batteries.

Severe shuttle effect of soluble polysulfides and sluggish redox kinetics have been thought of as the critical issues hindering the extensive applications of lithium-sulfur batteries (LSBs). Herein, one-dimensional boron nitride (1D BN) fibers with abundant pores and sufficient N-vacancy defects were synthesized using a thermal crystallization following a pre-condensation step. The 1D structure of BN facilitates unblocked ions diffusion pathways during charge/discharge cycles. The embedded pores within the polar BN strengthen the immobilization of polysulfides via both physical confinement and chemical interaction. Moreover, the highly exposed active surface area and intentionally created N-vacancy sites substantially promote reaction kinetics by lowering the energy barriers of the rate-limiting steps. After incorporating with conductive carbon networks and elemental S, the as-prepared S/Nv-BN@CBC cathode of LSBs deliver an initial discharge capacity of up to 1347 mAh g-1 at 200 mA g-1, while maintaining a low decay rate of 0.03 % per cycle over 1000 cycles at 1600 mA g-1. This work offers an effective strategy to mitigate the shuttle effect and highlights the significant potential of defect-engineered BN in accelerating the reaction kinetics of LSBs.

Universal design of three-dimensional porous graphene-iron based promotors for kinetically rationalized lithium-sulfur chemistry

Lithium-sulfur (Li-S) batteries are widely deemed to be one of the most potential candidates for future secondary batteries because of their remarkable energy density. Nevertheless, notorious polysulfide shuttling and retarded sulfur reaction kinetics pose significant obstacles to the further application of Li-S batteries. While rationally designed highly active electrocatalysts can facilitate polysulfide conversion, the universal and scalable synthesis strategies need to be developed. Herein, a universal synthetic strategy to construct a series of three-dimensional (3D) porous graphene-iron (3DGr-Fe) based electrocatalysts involving 3DGr-FeP, 3DGr-Fe3C, and 3DGr-Fe3Se4 is exploited for manipulating the Li-S redox reactions. It has been observed that the implementation of a 3D porous Gr architecture leads to the well-designed conductive networks, while the uniformly dispersed iron nanoparticles introduce an abundance of active sites, fostering the lithium polysulfide conversion, thereby bolstering the overall electrochemical performance. The Li-S battery with the 3DGr-Fe based electrocatalyst exhibits remarkable capacity retention of 94.8% upon 100 times at 0.2 C. Moreover, the soft-packaged Li-S pouch cell based on such a 3DGr-Fe electrocatalyst delivers superior capacity of 1060.71 mA h g−1 and guarantees for the continuous 30 min work of fan toy. This investigation gives comprehensive insights into the design, synthesis, and mechanism of 3DGr-Fe based electrocatalysts with high activity toward efficient and durable Li-S batteries.

Nitrogen-Doped Carbon and Metal-Nitrogen-Carbon Materials as Cathode Hosts for Li-S Batteries: Experimental Study and Mechanism Analysis.

Both nitrogen-doped carbon (NC) and metal-nitrogen-carbon (MNC) materials have been extensively investigated in lithium-sulfur batteries to alleviate the "shuttle effect". MNC are generally synthesized using NC as the parent material, wherein nitrogen atoms in NC serve as the "bridge" to coordinate with metal atoms. So far, an important scientific issue has not been settled: does the introduction of metal sites into NC certainly enhance the Li-S battery performance? In this work, NC and MNC materials derived from the same precursor, a nitrogen-rich porous polymer, are systematically compared as cathode hosts for Li-S battery through theoretical calculations and experimental investigation. Li-S cell with NC as the cathode sulfur host exhibits better cycle performance at low current densities (0.1 and 0.2C), whereas MNC materials predominate at higher current densities (such as 1C and 2C). Based on theoretical calculation and experimental results, it is concluded that the introduction of metal sites into NC through nitrogen bonding promoted the catalytic capability for faster sulfur redox reaction kinetics, whereas the adsorption energy toward polysulfides decreased. This work provides important guidance for more targeted design of advanced materials for lithium-sulfur battery application in the future.

Ultrathin titanium carbide-modified separator for high-performance lithium–sulfur batteries

Despite a high theoretical capacity, the practical application of lithium-sulfur batteries has been primarily limited by the migration of long-chained polysulfide species during the charge/discharge processes. One effective approach to address the issues is to design a functional separator or interlayer. Here, we prepared a modified separator with an ultrathin layer of titanium carbide (TiC) using radio-frequency sputtering on a commercial Celgard polypropylene membrane. The 240-nm TiC coating layer can enhance the interfacial properties of Celgard separators in porosity, wettability, roughness, etc. Hence, via experimental and theoretical investigation, we discovered that TiC can efficiently adsorb polysulfides and boost charge transfer via strong covalent C–S bonds. Using a TiC-modified separator can impede the shuttle effect and improve the kinetics of sulfur conversion reactions. Thus, the Li–S batteries with TiC separator deliver excellent electrochemical performances with a good rate capability (717 mAh g−1 at 7.0C) and an ultra-low decay rate of 0.058 % per cycle over 800 cycles at a C-rate of 2.0C. Furthermore, a high areal capacity of 4.3 mAh cm−2 was achieved with a high mass-loading of sulfur cathode up to 7.0 mg cm−2.

Amorphous bimetallic-organic framework enable accelerated redox kinetics and polysulfide trapping for lithium-sulfur batteries

Severe polysulfide dissolution and shuttling during charging and discharging are the main challenges hindering the practical application of lithium-sulfur (Li-S) batteries. Constructing functional separators is considered as an economical and convenient way to suppress the shuttle effect and improve the kinetics of Li-S chemistry. In this work, partially ligand-deficient amorphous bimetallic MOF material (aFeNi-MOF) is designed via a ligand competition strategy and employed as a separator modifier. The aFeNi-MOF not only promotes the rapid transportation of ions, but also enhances the chemisorption and catalytic capability on sulfur species, enabling accelerated redox kinetics and polysulfide trapping in Li-S batteries. Consequently, the assembled coin cell using aFeNi-MOF-modified separator delivered a high reversible capacity of 931.1 mAh/g at 1C, a long cycle life of more than 500 cycles and a low capacity decay of 0.084 % per cycle. Meanwhile, the areal capacity of 3.70 mAh cm−2 can be achieved under a high sulfur loading of 4.5 mg cm−2 and low electrolyte usage, meeting the requirement of areal capacity for commercial applications of Li-S batteries.