High Critical Current Density Research Articles

Pristine NASICON Electrolyte: A High Ionic Conductivity and Enhanced Dendrite Resistance Through Zirconia (ZrO2) Impurity-free Solid-Electrolyte Design.

Sodium batteries are considered a promising candidate for large-scale grid storage at tropical climate zone, and solid-state sodium metal batteries have a strong proposition as high energy density battery. The main challenge is to develop ultra-pure solid-state ceramic electrolyte and compatible metal interface. Here, a scalable and energy-efficient synthesis strategy of sodium (Na) Super Ionic CONductor, Na1+xZr2SixP3-xO12(x = 2, NZSP) solid electrolyte, has been introduced with the complete removal of unreacted zirconium oxide (ZrO2) impurities. Additionally, the reaction mechanism for the formation of pure phase NZSP is reported for the first time. The NZSP prepared by utilizing the Zr precursor, i.e., tetragonal zirconium oxide (t-ZrO2) derived from the Zr(OH)4 gets quickly and completely consumed in the synthesis process leaving no unreacted monoclinic ZrO2 impurities. The synthesis process only needs a minimum stay of 4 h, which is three times less than the conventional synthesis method. The elimination of ZrO2 impurities results in a 2.5-fold reduction in grain boundary resistivity, showcasing a total ionic conductivity of 1.75 mS cm-1 at room temperature and a relative density of 98%. The prepared electrolyte demonstrates remarkable resistance to dendrite formation, as evidenced by a high critical current density value of 1.4mA cm-2.

Boosting K+‐ionic Conductivity of Layered Oxides via Regulating P2/P3 Heterogeneity and Reciprocity for Room‐temperature Quasi‐solid‐state Potassium Metal Batteries

Solid‐state potassium metal batteries are promising candidates for grid‐scale energy storage due to their low cost, high energy density and inherent safety. However, solid state K‐ion conductors struggle with poor ionic conductivity due to the large ionic radius of K+‐ions. Herein, we report precise regulation of phase heterogeneity and reciprocity of the P2/P3‐symbiosis K0.62Mg0.54Sb0.46O2 solid electrolyte (SE) for boosting a high ionic conductivity of 1.6×10‐4 S cm‐1 at 25 °C. The bulk ionic conducting mechanism is explored by elucidating the effect of atomic stacking mode within the layered framework on K+‐ion migration barriers. For ion diffusion at grain boundaries, the P2/P3 biphasic symbiosis property assists in tunning the SE microstructure, which crystallizes in rod‐like particles with lengths of tens of micrometers facilitating long‐distance ion transport and significantly decreasing grain boundary resistance. Potassium metal symmetric cells using the modified SE deliver excellent cycling life over 300 h at 0.1 mA cm−2 and a high critical current density of 0.68 mA cm−2. The quasi‐solid‐state potassium metal batteries (QSSKBs) coupled with two kinds of layered oxide cathodes demonstrate remarkable stability over 300 cycles, outperforming the liquid electrolyte counterparts. The QSSKB system provides a promising strategy for high‐efficiency, safe, and durable large‐scale energy storage.

Boosting K+-ionic Conductivity of Layered Oxides via Regulating P2/P3 Heterogeneity and Reciprocity for Room-temperature Quasi-solid-state Potassium Metal Batteries.

Solid-state potassium metal batteries are promising candidates for grid-scale energy storage due to their low cost, high energy density and inherent safety. However, solid state K-ion conductors struggle with poor ionic conductivity due to the large ionic radius of K+-ions. Herein, we report precise regulation of phase heterogeneity and reciprocity of the P2/P3-symbiosis K0.62Mg0.54Sb0.46O2 solid electrolyte (SE) for boosting a high ionic conductivity of 1.6×10-4 S cm-1 at 25 °C. The bulk ionic conducting mechanism is explored by elucidating the effect of atomic stacking mode within the layered framework on K+-ion migration barriers. For ion diffusion at grain boundaries, the P2/P3 biphasic symbiosis property assists in tunning the SE microstructure, which crystallizes in rod-like particles with lengths of tens of micrometers facilitating long-distance ion transport and significantly decreasing grain boundary resistance. Potassium metal symmetric cells using the modified SE deliver excellent cycling life over 300 h at 0.1 mA cm-2 and a high critical current density of 0.68 mA cm-2. The quasi-solid-state potassium metal batteries (QSSKBs) coupled with two kinds of layered oxide cathodes demonstrate remarkable stability over 300 cycles, outperforming the liquid electrolyte counterparts. The QSSKB system provides a promising strategy for high-efficiency, safe, and durable large-scale energy storage.

Local plastic deformation effects on the critical current of high-Jc Nb3Sn strands under uniaxial strain

Abstract In order to meet the target operating parameters of the toroidal field coils (TFC) for the next-generation Chinese compact burning plasma tokamak, high critical current density (Jc) Nb3Sn strand will be applied to the high-field winding-package (WP) of the TFC. To improve the transverse stiffness of the cable in withstanding the huge Lorentz force and avoiding conductor performance degradation, the Short-Twist-Pitch (STP) and Copper-Wound-Strand (CWS) cable patterns were taken into consideration. In the processes of cabling and compaction of the conductor, the tight cable configurations lead to severe local plastic deformation (LPD) within the strands. The strands in the conductor are subjected to strain caused by thermal contraction and Lorentz force during conductor cooling down and operation. So far it is unknown, whether the LPD could impact the critical current (Ic) versus uniaxial applied strain behaviour of high-Jc Nb3Sn strand. Aiming to investigate the effect of LPD on the Ic of strands under uniaxial strain, three types of high Jc Nb3Sn strand with different indentation depths were tested on a U-shaped bending spring. The axial strain ranges from -0.9% to +0.4% at 14 T and 4.2 K. The three types of strands showed more strain sensitivity and lower tensile irreversible strain limit with increasing LPD, while even irreversible degradation of the Ic could be observed in the compressive strain region. The sample preparation, test process, test results and analysis are reported.

Controlled growth of YBCO film with tungsten oxide buffered substrate

This study explores the influence of tungsten oxide (WO3-x) nanostructures, decorated on LaAlO3 (LAO) single crystal substrate, on the fabrication and superconducting performance of YBa2Cu3Oy (YBCO) films. The WO3-x in square-dot and nanowire forms, significantly enhance the biaxial texture of YBCO films, resulting in high critical current density Jc (square-dot, 3.05 MA/cm2 @ 77 K, nanowire, 2.1 MA/cm2 @ 77 K). However, the presence of WO3-x nanodots leads to a random nucleation of YBCO grains along the a/b-axis, driving a porous surface and broadening the full width at half maximum (FWHM) in both phi and omega scans. This poor texture deteriorates the film’s Jc to 0.71 MA/cm2 @ 77 K. Therefore, optimizing the WO3-x interface is crucial for enhancing the epitaxial growth and critical current density of YBCO film. This study provides an effective approach to optimize the superconducting performance of YBCO film by tailoring nanostructure interface.

Construction of flexible asymmetric composite polymer electrolytes for high-voltage lithium metal batteries with superior performance

The primary obstacle hindering the application of composite solid electrolytes lies in the varying demands posed by the Li metal anode and the cathode, which needs to be capable of suppressing dendrite growth and resisting high voltage simultaneously. In this work, a new asymmetric composite solid-state electrolyte prepared via electrospinning and in-situ polymerization is proposed to address these shortcomings. In this bilayer architecture, polyacrylonitrile (PAN) layer of high-voltage tolerance, polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) layer of robust mechanical strength and good compatibility towards Li-anode are constructed, and metal-organic-frameworks (MOFs) are pre-embedded within both layers. The unique design provides a wide electrochemical stability window meanwhile ensures uniform lithium deposition. Remarkably, it exhibits a superior lithium utilization of 41 mAh cm−2 using a lean polymer electrolyte precursor and a high critical current density of 2.2 mA cm−2 with a thickness of 40 μm. Beneficial from the formation of a self-adjustable gradient solid electrolyte interphase in the Li/PVDF-HFP interface, the asymmetric electrolyte endows Li||Li and Li||NCM811 cells with excellent cycling stability. Moreover, the solid-state pouch cell exhibits reliable operation under extreme conditions. This work provides inspiration for the design and fabrication of composite solid electrolytes for next-generation high-voltage Li metal batteries.

Intercepting Dendrite Growth With a Heterogeneous Solid Electrolyte for Long-Life All-Solid-State Lithium Metal Batteries.

The application of lithium metal anode in all-solid-state batteries has the potential to achieve both high energy density and safety performance. However, the presence of serious dendrite issues hinders this potential. Here, the ion transport pathways and orientation of dendrite growth are regulated by utilizing the differences of ionic conductivity in heterogeneous electrolytes. The in situ formed Li-Ge alloy phases from the spontaneous reaction between Li10GeP2S12 and the attracted dendrites greatly enhance the ability to resist dendrite growth. As an outcome, the heterogeneous electrolyte achieves a high critical current density of 2.1mA cm-2 and long-term stable symmetrical battery operation (0.3mA cm-2 for 17000h and 1.0mA cm-2 for 2000h). Besides, due to the superior interfacial stability and low interface impedance between the heterogeneous electrolyte and lithium anode, the Li||LiNi0.8Co0.1Mn0.1O2 full battery exhibits great cycling stability (80.5% after 500 cycles at 1.0mA cm-2) and rate performance (125.4 mAh g at 2.0mA cm-2). This work provides a unique strategy of interface regulation via heterogeneous electrolytes design, offering insights into the development of state-of the-art all-solid-state batteries.

Constructing a three-dimensional continuous grain boundary with lithium ion conductivity and electron blocking property in LLZO to suppress lithium dendrites

Li7La3Zr2O12 (LLZO) stands out as a promising material for solid-state batteries due to its superior performance. However, the lithium dendrite growth in LLZO significantly affects battery performance due to high electronic conduction of LLZO. Herein, amorphous Li3BO3 (ALBO) is introduced into LLZO to construct a three-dimensional continuous grain boundary with lithium ion conductivity and electron-blocking property to suppress lithium dendrites. The symmetric cells of ALBO-LLZO achieved a high critical current density (CCD) of 1.1 mA·cm−2 and cycled stably for 2000 h at 0.3 mA·cm−2. The capacity retention of LFP/1 ALBO-LLZO/Li battery retains 84.6 % after 200 cycles at 0.2 C, room temperature. This research offers a potential solution to enhance the performance of the garnet electrolyte for ASSBs.

Quadrupling the depairing current density in the iron-based superconductor SmFeAsO1-xHx.

Iron-based 1111-type superconductors display high critical temperatures and relatively high critical current densities Jc. The typical approach to increasing Jc is to introduce defects to control dissipative vortex motion. However, when optimized, this approach is theoretically predicted to be limited to achieving a maximum Jc of only ∼30% of the depairing current density Jd, which depends on the coherence length and the penetration depth. Here we dramatically boost Jc in SmFeAsO1-xHx films using a thermodynamic approach aimed at increasing Jd and incorporating vortex pinning centres. Specifically, we reduce the penetration depth, coherence length and critical field anisotropy by increasing the carrier density through high electron doping using H substitution. Remarkably, the quadrupled Jd reaches 415 MA cm-2, a value comparable to cuprates. Finally, by introducing defects using proton irradiation, we obtain high Jc values in fields up to 25 T. We apply this method to other iron-based superconductors and achieve a similar enhancement of current densities.

Nonstoichiometry Induced Amorphous Grain Boundary of Na5SmSi4O12 Solid-State Electrolyte for Long-Life Dendrite-Free Sodium Metal Battery.

Oxide ceramics are considered promising candidates as solid electrolytes (SEs) for sodium metal batteries. However, the high sintering temperature induced boundaries and pores between angular grains lead to high grain boundary resistance and pathways for dendrite growth. Herein, we report a grain boundary modification strategy, which in situ generates an amorphous matrix among Na5SmSi4O12 oxide grains via tuning the chemical composition. The mechanical properties as well as electron mitigating capability of modified SE have been significantly enhanced. As a result, the SE achieves a room-temperature total ionic conductivity of 5.61 mS cm-1, the highest value for sodium-based oxide SEs. The Na|SE|Na symmetric cell achieves a high critical current density of 2.5 mA cm-2 and excellent cycle life over more than 2800 h at 0.15 mA cm-2 without dendrite formation. The full cell with Na3V2(PO4)3 as the cathode demonstrates impressive cycling performance, maintaining stability over 3000 cycles at 5C without observable loss of capacity.

Structural properties of LATP ceramic pellets sintered at 900 °C and modified by a novel solution-immersion densification process

The high temperature sintered ceramic pellets of solid electrolyte Li1.3Al0.3Ti1.7(PO4)3 (LATP), obtained in the absence of any sintering aids, should contain a large amount of interparticle gaps, which is one of the main bottlenecks in developing LATP-based all-solid-state Li-metal batteries. In this study, a facile solution (LiCl in ethanol) immersion method is adopted to soak the already 900℃-sintered LATP ceramic pellets, and the resulting series of LATP-xLiCl (x denotes the weight fraction of LiCl, 0.0 ≤ x ≤ 3.7) are assayed to address the high-performance mechanism of lithium-graphite (Li-C) symmetric cells. At the optimal x value of 2.3, the grain-boundary resistance of the ceramic pellet can be significantly reduced from 1772 to 28 Ω·cm² at room temperature, which endows the Li-C symmetrical cells of LATP-2.3LiCl with a high critical current density of 3.00 mA cm² at 60°C. Especially, the enhanced ionic conductivity of LATP-2.3LiCl (4.7×10−4 S cm−1, at 20℃; 1.1×10−3 S cm−1, at 60℃) indicates an effective strategy of utilizing capillary force to densify LATP-based ceramic pellets for potential application purposes.

Bonded Interface Enabled Durable Solid‐state Lithium Metal Batteries with Ultra‐low Interfacial Resistance of 0.25 Ω cm2

AbstractThe solid‐state batteries (SSBs) with Li anode present one of the most promising energy storage systems due to their enhanced energy density and safety. However, interfacial problems between Li anode and solid‐state electrolyte hinder the advancement of SSBs. Among them, insufficient solid‐solid interfacial contact is the main issue, which causes large resistance and hinders Li+ diffusion, leading to current distribution unevenness and lithium dendrites growth. To meet these challenges, a silver/carbon interlayer composed of ultrafine Ag nanoparticles (≈5 nm) grown on COOH‐CNTs (nano‐Ag@COOH‐CNTs) is constructed. In which, nano‐Ag is designed to guide homogeneous Li deposition, while CNTs substrate bonds with Li6.5La3Zr1.5Ta0.5O12 (LLZTO) electrolyte by reactions between ─COOH groups and LLZTO alkaline surface, thus transforming loose physical solid‐solid contact to chemical bonding contact. In addition, nano‐Ag is immobilized by CNTs, avoiding the migration of Li+ implanted nano‐Ag during cycling. Therefore, nano‐Ag@COOH‐CNTs interlayer can boost Li+ transport at LLZTO/Li interface and inhibit Li dendrites, achieving an ultra‐low interfacial resistance of 0.25 Ω cm2, a high critical current density of 1.7 mA cm−2 and a long cycling over 2155 h at 0.5 mA cm−2. The modified SSBs with LiNi0.83Co0.12Mn0.05O2 cathode cycles stably over 500 cycles. Moreover, high‐loading SSBs operate stably for 85 cycles.

Fabrication of microstrips of iron-based superconductor NdFeAs(O,H)

NdFeAs(O,H) microstrips with line widths of about 1–5 µm were fabricated by photolithography and Ar-ion dry etching. The microstrips were fabricated under two different etching conditions: 25 min etching at a power of 20 W (long duration, low power) and 3 min etching at 100 W (short duration, high power). For both conditions, the narrowest microstrips, which were 0.9 µm in width, retained high critical temperatures of about 85% of those before microfabrication. Further, the 0.9 µm microstrip fabricated under the high-power, short-duration condition exhibited a high critical current density (J c) of more than 4 MA cm−2 at 4 K. However, J c of the microstrip fabricated under the low-power, long-duration condition was somewhat lower. Our analysis suggests that the edges of the microstrips were damaged more than twice as wide as those of the microstrips fabricated under the high-power, short-duration condition. This indicates that a short duration is more effective to reduce the damage than using a lower etching power.

Zwitterionic Cellulose-Based Polymer Electrolyte Enabled by Aqueous Solution Casting for High-Performance Solid-State Batteries.

Polyethylene oxide (PEO)-based solid-state batteries hold great promise as the next-generation batteries with high energy density and high safety. However, PEO-based electrolytes encounter certain limitations, including inferior ionic conductivity, low Li+ transference number, and poor mechanical strength. Herein, we aim to simultaneously address these issues by utilizing one-dimensional zwitterionic cellulose nanofiber (ZCNF) as fillers for PEO-based electrolytes using a simple aqueous solution casting method. Multiple characterizations and theoretical calculations demonstrate that the unique zwitterionic structure imparts ZCNF with various functions, such as disrupting PEO crystallization, dissociating lithium salts, anchoring anions through cationic groups, accelerating Li+ migration by anionic groups, as well as its inherent reinforcement effect. As a result, the prepared PL-ZCNF electrolyte exhibits remarkable ionic conductivity (5.37×10-4 S cm-1) and Li+ transference number (0.62) at 60 °C without sacrificing mechanical strength (9.2 MPa), together with high critical current density of 1.1 mA cm-2. Attributed to these merits of PL-ZCNF, the LiFePO4|PL-ZCNF|Li solid-state full-cell delivers exceptional rate capability and cycling performance (900 cycles at 5 C). Notably, the assembled pouch-cell can maintain steady operation over 1000 cycles with an impressive 93.7 % capacity retention at 0.5 C and 60 °C, highlighting the great potential of PL-ZCNF for practical applications.

Zwitterionic Cellulose‐Based Polymer Electrolyte Enabled by Aqueous Solution Casting for High‐Performance Solid‐State Batteries

AbstractPolyethylene oxide (PEO)‐based solid‐state batteries hold great promise as the next‐generation batteries with high energy density and high safety. However, PEO‐based electrolytes encounter certain limitations, including inferior ionic conductivity, low Li+ transference number, and poor mechanical strength. Herein, we aim to simultaneously address these issues by utilizing one‐dimensional zwitterionic cellulose nanofiber (ZCNF) as fillers for PEO‐based electrolytes using a simple aqueous solution casting method. Multiple characterizations and theoretical calculations demonstrate that the unique zwitterionic structure imparts ZCNF with various functions, such as disrupting PEO crystallization, dissociating lithium salts, anchoring anions through cationic groups, accelerating Li+ migration by anionic groups, as well as its inherent reinforcement effect. As a result, the prepared PL‐ZCNF electrolyte exhibits remarkable ionic conductivity (5.37×10−4 S cm−1) and Li+ transference number (0.62) at 60 °C without sacrificing mechanical strength (9.2 MPa), together with high critical current density of 1.1 mA cm−2. Attributed to these merits of PL‐ZCNF, the LiFePO4|PL‐ZCNF|Li solid‐state full‐cell delivers exceptional rate capability and cycling performance (900 cycles at 5 C). Notably, the assembled pouch‐cell can maintain steady operation over 1000 cycles with an impressive 93.7 % capacity retention at 0.5 C and 60 °C, highlighting the great potential of PL‐ZCNF for practical applications.

High-Strength, Thin, and Lightweight Solid Polymer Electrolyte for Superior All-Solid-State Sodium Metal Batteries.

The utilization of solid polymer electrolytes (SPEs) in all-solid-state sodium metal batteries has been extensively explored due to their excellent flexibility, processability adaptability to match roll-to-roll manufacturing processes, and good interfacial contact with a high-capacity Na anode; however, SPEs are still impeded by their inadequate mechanical strength, excessive thickness, and poor stability with Na anodes. Herein, a robust, thin, and cost-effective polyethylene (PE) film is employed as a skeleton for infiltrating poly(ethylene oxide)-sodium bis(trifluoromethanesulfonyl)imide (PEO/NaTFSI) to fabricate PE-PEO/NaTFSI SPE. The resulting SPE features a remarkable thickness of 25 μm, lightweight property (2.1 mg cm-2), superior mechanical strength (tensile strength = 100.3 MPa), and good flexibility. The SPE also shows an ionic conductivity of 9.4 × 10-5 S cm-1 at 60 °C and enhanced interfacial stability with a sodium metal anode. Benefiting from these advantages, the assembled Na-Na symmetric cells with PE-PEO/NaTFSI show a high critical current density (1 mA cm-2) and excellent long-term cycling stability (3000 h at 0.3 mA cm-2). The all-solid-state Na||PE-PEO/NaTFSI||Na3V2(PO4)3 coin cells exhibit a superior cycling performance, retaining 93% of the initial capacity for 190 cycles when matched with a 6 mg cm-2 cathode loading. Meanwhile, the pouch cell can work stably after abuse testing, proving its flexibility and safety. This work offers a promising strategy to simultaneously achieve thin, high-strength, and safe solid-state electrolytes for all-solid-state sodium metal batteries.

In Situ Fabrication of High Ionic and Electronic Conductivity Interlayers Enabling Long-Life Garnet-Based Solid-State Lithium Batteries.

Garnet-type Li6.75La3Zr1.75Ta0.25O12 (LLZTO) is a promising solid-state electrolyte (SSE) because of its fast ionic conduction and notable chemical/electrochemical stability toward the lithium (Li) metal. However, poor interface wettability and large interface resistance between LLZTO and Li anode greatly restrict its practical applications. In this work, we develop an in situ chemical conversion strategy to construct a highly conductive Li2S@C layer on the surface of LLZTO, enabling improved interfacial wettability between LLZTO and the Li anode. The Li/Li2S@C-LLZTO-Li2S@C/Li symmetric cell has a low interface impedance of 78.5 Ω cm2, much lower than the 970 Ω cm2 of a Li/LLZTO/Li cell. Moreover, the Li/Li2S@C-LLZTO-Li2S@C/Li cell exhibits a high critical current density of 1.4 mA cm-2 and an ultralong stability of 3000 h at 0.1 mA cm-2. When used in a LiFePO4 battery, the Li/Li2S@C-LLZTO/LiFePO4 battery exhibits a high initial discharge capacity of 150.8 mA h g-1 at 0.2 C without lithium storage capacity attenuation during 200 cycles. This work provides a novel and feasible strategy to address interface issues of SSEs and achieve lithium-dendrite-free solid-state batteries.

Removal and Reoccurrence of LLZTO Surface Contaminants under Glovebox Conditions.

The reactivity of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) solid electrolytes to form lithio-phobic species such as Li2CO3 on their surface when exposed to trace amounts of H2O and CO2 limits the progress of LLZTO-based solid-state batteries. Various treatments, such as annealing LLZTO within a glovebox or acid etching, aim at removing the surface contaminants, but a comprehensive understanding of the evolving LLZTO surface chemistry during and after these treatments is lacking. Here, glovebox-like H2O and CO2 conditions were recreated in a near ambient pressure X-ray photoelectron spectroscopy chamber to analyze the LLZTO surface under realistic conditions. We find that annealing LLZTO at 600 °C in this atmosphere effectively removes the surface contaminants, but a significant level of contamination reappears upon cooling down. In contrast, HCl(aq) acid etching demonstrates superior Li2CO3 removal and stable surface chemistry post treatment. To avoid air exposure during the acid treatment, an anhydrous HCl solution in diethyl ether was used directly within the glovebox. This novel acid etching strategy delivers the lowest lithium/LLZTO interfacial resistance and the highest critical current density.

Superior Superconducting Properties Realized in Quaternary La-Y-Ce Hydrides at Moderate Pressures.

The recent revolution in the superconductivity field stems from hydride superconductors. Multicomponent hydrides provide a crucial platform for tracking high-temperature superconductors. Besides high superconducting transition temperature (Tc), achieving both giant upper critical magnetic field [μ0Hc2(0)] and high critical current density [Jc(0)] is also key to the latent potential of the application for hydride superconductors. In this work, we have successfully synthesized quaternary La-Y-Ce hydrides with excellent properties under moderate pressure by using the concept of "entropy engineering." The obtained temperature dependence of the resistance provides evidence for the superconductivity of Fm3m-(La,Y,Ce)H10, with the maximum Tc ∼ 190 K (at 112 GPa). Notably, Fm3m-(La,Y,Ce)H10 boasts exceptional properties: μ0Hc2(0) reaching 292 T and Jc(0) surpassing 4.61 × 107 A/cm2. Compared with the binary LaH10/YH10, we find that the Fm3m structure in (La,Y,Ce)H10 can be stable at relatively low pressures (112 GPa). These results indicate that multicomponent hydrides can significantly enhance the superconducting properties and regulate stabilizing pressure through the application of "entropy engineering." This work stimulates the experimental exploration of multihydride superconductors and also provides a reference for the search of room-temperature superconductors in more diversified hydride materials in the future.

Interfacial Design Strategy for Polymeric Lithium Metal Batteries with Superfast Charge‐Transfer Kinetics

AbstractInterfacial instability including the high charge‐transfer resistance and the uncontrolled lithium dendrite growth have severely restricted the safety, fast‐charging, and high‐power capabilities of solid‐state polymeric lithium metal batteries (PLMBs). Here, the study demonstrates the ionic nanoclusters self‐assembled between the lithium ions and a rigid‐rod sulfonated aromatic polyamide Poly 2,2′‐disulfonyl‐4,4′‐benzidine terephthalamide (PBDT) can facilitate uniform lithium deposition; meanwhile, realizing 102–103 times lower interfacial charge‐transfer resistance than PEO‐based electrolytes and excellent lithium dendrite suppression at the interfaces. The cells assembled with this solid‐state polymer electrolyte at room temperature show a record high critical current density (6 mA cm−2/3 mAh cm−2), 80% capacity retention at 10 000 cycles (5 C) with the LiFePO4 cathode. With the temperature increased to 80 °C, the cells enable almost 100% of the theoretical capacity at 3 C and high specific power density (20 kW kg−1). According to the Cryo‐TEM imaging and computational simulation results, it is concluded that these nanoscale self‐assembled ionic nanoclusters play a critical role in realizing the superfast charge‐transfer kinetics by balancing the pre‐exponential factor and activation energy at the lithium‐polymer space‐charge interfaces. This interfacial design strategy based on thermodynamically favored ion‐association and self‐assembly between the metal ions and the polyanions guarantees superior charge‐transfer kinetics in PLMBs.