Li Salt Research Articles

Suppressing Interfacial Side Reactions of Anode-Free Lithium Batteries by an Organic Salt Monolayer.

Anode-free lithium (Li) batteries are attractive owing to their high energy density. However, Li loss by forming solid-electrolyte interphase (SEI) during cell activation leads to a ≈25% capacity decrease, and the capacity constantly fades upon cycling due to the side reactions on the copper (Cu) current collector. This paper reports high-initial-efficiency, long-cycle-life, and long-calendar-life anode-free Li batteries by using an organic Li salt monolayer bonded on Cu. The functional salt, namely lithium ((4-carbamoylphenyl)sulfonyl)(fluorosulfonyl)imide, electrochemically decomposes and passivates the Cu surface, which reduces Li sacrifice by SEI formation and suppresses galvanic Li corrosion and Li-electrolyte reactions during cycling. This work records a LiF-rich interphase on Cu and guided Li nucleation and growth. A 93.6% initial Li deposition efficiency is realized in a regular carbonate electrolyte, and the galvanic current is decreased to ≈40 nA cm-2 , merely one-tenth of bare Cu. After cell activation, 95.2% capacity is retained for a Cu|LiNi0.8 Mn0.1 Co0.1 pouch cell with a theoretical capacity of 200 mAh, and the cell is operated over 600 cycles. Calendar aging showed no damage to cell performance.

Integration Plasma Strategy Controlled Interfacial Chemistry Regulation Enabling Planar Lithium Growth in Solid‐State Lithium Metal Batteries

AbstractSolid‐state lithium metal batteries (SSLMBs) are identified as a highly promising candidate for next‐generation energy storage devices, yet they still face uncontrollable dendritic lithium (Li) growth originating from interfacial incompatibility. To address this issue, an “integration plasma (IP)” strategy for interlayer construction is proposed that integrates metal reduction and vapor deposition functions, featuring the ability to give a manipulable and quantifiable chemical regulation for controlling the surface concentration (Csurface) and the atomic ratio of the introduced metal element and electronegative element (ARE/M) on solid‐state electrolyte (SSE). This IP‐formed interlayer can in situ react with Li anode to synchronously produce metal‐Li alloy, Li salt and amorphous carbon, thus offering an “integrated function” to promote a spherical and hexagonal Li growth, preventing the dendrite propagation from SSE. When Csurface of metal elements and corresponding ARE/M is regulated as ≈1.13 nmol cm‐2 and ≈2.6, the IP‐modified SSE prolongs the lifespan of SSLMBs with LiNi0.8Co0.1Mn0.1O2 cathode to over 1000 cycles with a low‐capacity attenuation of 0.03% per cycle, highlighting the multiply functions of IP to accelerate the practical application of SSLMBs.

Eco‐Friendly Tetrahydropyran Enables Weakly Solvating “4S” Electrolytes for Lithium‐Metal Batteries

AbstractThe growth of lithium dendrites hinders the commercial applications of lithium‐metal batteries. Electrolytes play a crucial role in influencing electrode/electrolyte interfacial chemistry. Traditional electrolytes adopt strongly solvating solvents to dissolve Li salts, creating an organic‐rich solid electrolyte interface (SEI). The Li+ conductivity and mechanical strength of the organic‐rich SEI are poor, so the derived SEI cannot effectively suppress the growth of Li dendrites. The weakly solvating electrolyte (WSE) system can realize an inorganic‐rich SEI, demonstrating improved compatibility with the Li metal. However, the design rules for the WSE are not clear. Here, four kinds of “4S” (single salt and single solvent) WSE are designed to investigate interface chemistry. The SEI thickness, pore volume, and porosity are revealed via a reactive force field. The results show the heterocyclic and symmetric tetrahydropyran has the most suitable solvating power and the best interfacial stability in the lithium‐metal battery system. This research provides a weakly solvating electrolyte design route for bridging the molecular thermodynamic and interfacial chemistry gap.

Tunable all-solid-state wire-shaped high power device based on carbon nanotubes yarn

Energy storage devices integrated into textiles have emerged as a significant strategy for electronic applications. In this context, in the present paper novel flexible devices were developed, in which the control of both the electrode characteristics and the solid-electrolyte properties allows to build all-solid-state wire-shaped supercapacitors that can be integrated and waved. The proposed device was assembled using modified CNT yarns as electrodes and a blend of ionic liquid, Li salt and poly(ethylene glycol) acrylate to fabricate the solid-polymeric electrolyte. Excellent performance in terms of both electrochemical parameters and stability were obtained. These achievements are possible thanks to the coupling of asymmetric CNT yarns, following an optimization of the activation procedure together with the improvement of the polymeric electrolyte. The results show a capacitance as high as 1.8 mF/cm, energy density of 1.3 μWh/cm and a capacitance retention higher than 100% over 1200 cycles.

Coupled Ion-Conduction Mechanism for Enhanced Ionic Conductivity in Mg2B2O5 Nanowires Enabled Poly(ethylene oxide)-Based Quasi Solid State Electrolytes

Achieving room temperature high ionic conductivity of polymer solid state electrolytes equivalent to organic liquid electrolytes currently used in lithium ion batteries is a challenging task. The glass transition, crystallinity, free volume structure, salt dissociation, and ionic diffusion affect the ionic conductivity of polymer-based solid state electrolytes. In the present study, we report high-ionic conductivity (4.1 × 10–4 Scm–1) at room temperature for Mg2B2O5 nanowire-enabled solid state electrolytes of fully amorphous poly(ethylene oxide) (PEO). The Mg2B2O5 nanowires are synthesized using a single-step solid state reaction from inexpensive materials. The detailed investigation of the ion conduction mechanism using broadband dielectric spectroscopy confirms that the ionic conduction and segmental relaxations are a coupled phenomenon in these electrolytes, and segmental relaxation-mediated ionic diffusion is the primary ionic conduction mechanism. The enhancement in ionic conductivity on loading of Mg2B2O5 nanowires is attributed to the enhancement in the dissociated ionic concentration, ionic diffusion, and faster segmental relaxation due to interactions between the polymer, Li salt, and the nanowires. The smaller free volume size and enhanced free volume density of PEO in the electrolytes determined using positron annihilation lifetime spectroscopy and reduction in glass transition temperature determined from differential scanning calorimetry further confirm the role of modified chain packing and segmental relaxations in enhancement of ionic conductivity.

PEO-based solid-state electrolyte modified by cationic covalent organic frameworks enabling high-performance all-solid-state Li metal and graphite anode batteries

Covalent organic frameworks (COFs) with regular and ordered channels have been proved that they could offer extra space to accommodate ions and fast conduction pathways for ion motion. However, the ion conductivities of their own are not high because of most of them have no enough active segmental motion of polymer chains for ion transport. Polyethylene oxide (PEO) is the most typical and efficient solid-state polymer material for Li+ migration by the segmental motion of molecular chains. Herein, we propose a simple and effective strategy of introducing a small quantity of cationic COF additive EB-COF-TFSI into the PEO of low glass transition temperature to obtain high-performance solid-state electrolyte (SSEs) and Li batteries. The cationic COF structure not only provides fast pathway for Li+ but also these cations on it accelerate Li salt dissociation and Li+ conduction. As a result, the cycling time of Li symmetrical cells increases to triplication at a same test condition; the corresponding all-solid-state LFP and NMC//Li metal cells are stimulated to release higher specific capacities, exhibit an enhanced cycling stability and better rate capability. It is surprising that all-solid-state LFP//graphite cells show excellent charging and discharging performance no matter on longtime cycling or rate performance test which are both much better than that of Li metal cells and provide a great strategy for building commercial all-solid-state Li battery based the current structure of it.

Synthesis and Electrochemical Properties of Electrolytes Based on Phosphonium, Sulfonium and Imidazolium Ionic Liquids for Li-Ion Batteries

This work describes synthesis and characterization of three ionic liquids (IL) with imidazolium, phosphonium or sulfonium cations. These ILs were used as precursors for the preparation of electrolytes by adding various types of lithium salts. Thermal and electrochemical properties of the electrolytes were studied to assess their feasibility for usage in lithium-ion batteries (LIB). Ethylmethylimidazolium phosphonic acid ethyl ester [EtMeIm]+[EtPITE]– with added Li salts showed very low conductivities of about 0.02 mS cm–1 and a rather narrow electrochemical stability window of 4.3 V. Of all the ILs under study, this imidazolium-based IL exhibited the worst thermal properties both neat and with additional Li+ salt. Therefore, using this IL as an electrolyte for LIB is unlikely. Methyl­tributylphosphonium bis(trifluoromethyl sulfonyl) imide [P1444]+[TFSI]– with Li salts had already significantly higher conductivities of 0.4–0.6 mS cm–1 and showed a very wide electrochemical stability window of 7 V. TGA curves of [P1444]+[TFSI]– show excellent thermal stability up to 300 °C. DSC measurements showed semicrystalline behaviour of [P1444]+[TFSI]–; this unfavourable fact was overcome by the addition of Li+ salts. Potential of this IL is very high for the use in LIB. At room temperature, trimethylsulfonium bis(trifluoromethyl sulfonyl) imide [S111]+[TFSI]– is a solid crystalline material, so it was mixed with [P1444]+[TFSI]–. The resulting mixture [P1444]+[S111]+[TFSI]– achieved the highest conductivities of 0.6–1.0 mS cm–1 in comparison to other prepared ILs. The electrochemical stability is also interesting, its ESW value being 5.5 V. Thermal properties are comparable to those of [P1444]+[TFSI]–, but it does not show semicrystalline behaviour. This mixture is a promising electrolyte for LIB.
 Full text English translation is available in the on-line version.

Gel electrolyte with dimethyl sulfoxide confined in a polymer matrix for Li-air batteries operable at sub-zero temperature

The instability of the electrolyte and insufficient ionic conductivity are considered the main problems that adversely affect applications of Li-air batteries (LABs) at sub-zero temperatures. In this study, a polymer-confined gel (PCG) electrolyte suitable for low-temperature LABs is developed by confining high donor number dimethyl sulfoxide (DMSO) within an in situ polymerized 4,4′-bis(stearoylamino)diphenyl ether (BSDE) matrix. The strong hydrogen bonds between the BSDE framework and DMSO molecules has destroyed the frozen structure of DMSO, thus the ionic conductivity at lower temperature has thus been improved. Furthermore, a local high-concentration electrolyte is constructed using DMSO as a solvent to dissolve the Li salt. The ionic conductivity of PCG in the fabricated electrolyte at −20 °C is maintained at 0.15 mS cm−1, which is 5.5 times higher than the corresponding liquid DMSO electrolyte. As a result, the LABs equipped with PCG display a long cycle life of 450 h (−20 °C) and 760 h (25 °C), whereas the LABs with a liquid DMSO electrolyte fail at −20 °C and can only operate for 40 h at 25 °C. This study provides a feasible but facile strategy for the design of gel electrolytes suitable for low-temperature LABs, and this strategy can be extended to other energy-storage systems.

A medium/low concentration localized electrolyte for safe and fast-charging lithium-ion batteries

Localized high concentrations electrolyte (LHCE) has garnered significant attention as an emerging electrolyte candidate for Li-metal batteries. LHCE is formed by diluting a high concentration electrolyte (usually close to saturation) with a non-solvating solvent that has a low donor number. We propose a modified concept of LHCE, called "localized electrolyte (LE)," optimized for Li-ion batteries with a graphite anode and Ni-rich cathode. In LE, the Li salt concentration is optimized to be only 1-2 M in solvating solvents, resulting in an overall concentration of 0.5–1 M, which reduces cost and supports fast ion transport. The non-flammable LE also has excellent wettability, which facilitates fasting charging. We also demonstrated that with the addition of 2 wt.% vinylene carbonate into 0.7 M LE, the Li-ion cell retains 80.3% of its initial capacity after 700 cycles of testing in about 4 months. Overall, LE represents a promising and cost-effective solution for improving the performance and safety of Li-ion batteries.

A Molecularly Engineered Cathode Lithium Compensation Agent for High Energy Density Batteries.

Prelithiating cathode is considered as one of the most promising lithium compensation strategies for practical high energy density batteries. Whereas most of reported cathode lithium compensation agents are deficient owing to their poor air-stability, residual insulating solid, or formidable Li-extracting barrier. Here, this work proposes molecularly engineered 4-Fluoro-1,2-dihydroxybenzene Li salt (LiDF) with high specific capacity (382.7 mAh g-1 ) and appropriate delithiation potential (3.6-4.2V) as an air-stable cathode Li compensation agent. More importantly, the charged residue 4-Fluoro-1,2-benzoquinone (BQF) can synergistically work as an electrode/electrolyte interface forming additive to build uniform and robust LiF-riched cathode/anode electrolyte interfaces (CEI/SEI). Consequently, less Li loss and retrained electrolyte decomposition are achieved. With 2wt% 4-Fluoro-1,2-dihydroxybenzene Li salt initially blended within the cathode, 1.3 Ah pouch cells with NCM (Ni92) cathode and SiO/C (550 mAh g-1 ) anode can keep 91% capacity retention after 350 cycles at 1 C rate. Moreover, the anode free of NCM622+LiDF||Cu cell achieves 78% capacity retention after 100 cycles with the addition of 15wt% LiDF. This work provides a feasible sight for the rational designing Li compensation agent at molecular level to realize high energy density batteries.

Electrolyte strategy toward the low-temperature Li-metal secondary battery

Lithium metal battery (LMB) always faces a huge challenge at low temperature due to the sluggish reaction kinetics. An effective electrolyte could well tackle the issues as it much determines the Li+ de-solvation behavior and solid electrolyte interface (SEI) formation, and further greatly influenced the Li deposition. A practicable and cost-effective electrolyte was proposed in this work which sophisticatedly handled the balance between the ion-transfer character, Li solvation and SEI requirement. Highly fluent methyl acetate (MA) and SEI-beneficial fluoroethylene carbonate (FEC) together with Li salt constituted an anti-freezing electrolyte with sufficient ion-conductivity. More importantly, appropriate coordination between salt and solvent facilitated the de-solvation stage in Li+-reduction, additionally, the dual salt of lithium bis(fluorosulfonyl)imide (LiFSI) and lithium difluoro(oxalate)borate (LiODFB) combining with LiNO3 additive endowed the electrolyte with wide electrochemical window and Al compatibility. With them, repetitive Li striping/plating was achieved at −40 °C, and Li/LiNi0.5Co0.2Mn0.3O2 (NCM) full cell could be stably cycled for more than 150 times.

Effect of nano Al2O3 addition on cycling performance of poly(ether block amide) based solid-state lithium metal batteries

A novel poly(ether block amide) (PEBA) based solid-state polymer electrolyte (SPE) was prepared using a casting method, in which 20wt% lithium (Li) bis-(trifluoromethanesulfonyl)imide (LiTFSI) and aluminum oxide (Al2O3) nanoparticles were used as the Li salt and solid plasticizer, respectively. In the case of addition of 3wt% Al2O3 nanoparticles, ion conductivity of the obtained PEBA 2533–20wt% LiTFSI-3wt% Al2O3 SPE was 3.57 × 10−5 S cm−1 at 25 °C. Furthermore, the Li symmetrical battery assembled with it showed excellent cycling stability (1000 h) at 0.1 mA cm−2. While, the assembled all-solid-state Li/PEBA 2533–20% LiTFSI-3wt% Al2O3/LiFePO4 (areal capacity: 0.15 mAh cm−2) battery maintained 94.9% of the maximal capacity (133.9 mAh g−1@0.1 mA cm−2) at 60 °C even after 650 cycles with a superior average coulombic efficiency (CE) of 99.84%. By using X-ray photoelectron spectroscope (XPS), self-aggregation layer (SAL) of polyamide 12 (PA12) of PEBA 2533 was discovered, which should contribute to promoting the robustness of lithium fluoride (LiF) enriched solid-electrolyte interphase (SEI) layer. In addition, it is considered that the state of interface between SPE and cathode should be the cause of voltage polarization of the full cell.

Uncoordinated chemistry enables highly conductive and stable electrolyte/filler interfaces for solid-state lithium–sulfur batteries

Composite-polymer-electrolytes (CPEs) embedded with advanced filler materials offer great promise for fast and preferential Li+ conduction. The filler surface chemistry determines the interaction with electrolyte molecules and thus critically regulates the Li+ behaviors at the interfaces. Herein, we probe into the role of electrolyte/filler interfaces (EFI) in CPEs and promote Li+ conduction by introducing an unsaturated coordination Prussian blue analog (UCPBA) filler. Combining scanning transmission X-ray microscope stack imaging studies and first-principle calculations, fast Li+ conduction is revealed only achievable at a chemically stable EFI, which can be established by the unsaturated Co-O coordination in UCPBA to circumvent the side reactions. Moreover, the as-exposed Lewis-acid metal centers in UCPBA efficiently attract the Lewis-base anions of Li salts, which facilitates the Li+ disassociation and enhances its transference number (tLi+). Attributed to these superiorities, the obtained CPEs realize high room-temperature ionic conductivity up to 0.36 mS cm-1 and tLi+ of 0.6, enabling an excellent cyclability of lithium metal electrodes over 4,000 h as well as remarkable capacity retention of 97.6% over 180 cycles at 0.5 C for solid-state lithium-sulfur batteries. This work highlights the crucial role of EFI chemistry in developing highly conductive CPEs and high-performance solid-state batteries.

Effects of Molecular Structure of Cross-Linked Solid Polymer Electrolytes on Ionic Conduction Behavior

To improve the safety and energy density of Li batteries, all-solid-state batteries (ASSBs) are desired. Solid polymer electrolytes (SPEs) are expected to be promising candidates, owing to features such as their high flexibility and formability. To achieve high-performance ASSBs, we investigated molecular structure design by fabricating two types of SPEs. First, chemically cross-linked polyethylene oxide/polypropylene oxide (P(EO/PO))-based SPEs were formed with low-molecular-weight PEO as side chains. Second, physically cross-linked SPEs were fabricated with short PEO chains (G2) as soft-units and norbornene (NB) as hard-units with intramolecular phase separation. Evaluation of the physicochemical and electrochemical properties of these SPEs was carried out, and the degree of dissociation of the Li salt was investigated by Raman spectroscopy. The phenomenon of decoupling between the segmental motion of the SPEs and ionic conduction was confirmed by Vogel-Fulcher-Tamman equation analysis. P(NB/G2)-based SPEs also exhibited high thermal stability, which originated from the NB unit, according to TG-DTA and DSC measurements. Furthermore, ionic conductivity increased monotonically with the Li salt concentration, in contrast to conventional PEO-based SPEs. Physically cross-linked SPEs achieved the decoupling of ionic conduction from their segmental motion owing to their differences between the ionic and structural components of the SPEs.

Cooperative Proton and Li-ion Conduction in a 2D-layered MOF via Mechanical Insertion of Lithium Halides.

Ionic conduction in highly designable and porous metal-organic frameworks has been explored through the introduction of various ionic species (H+, OH-, Li+, etc.) using post-synthetic modification such as acid, salt, or ionic liquid incorporation. Here, we report on high ionic conductivity (σ > 10-2 S cm-1) in a two-dimensionally (2D)-layered Ti-dobdc (Ti2(Hdobdc)2(H2dobdc), H4dobdc: 2,5-dihydroxyterephthalic acid) via LiX (X= Cl, Br, I) intercalation using mechanical mixing. The anionic species in lithium halide strongly affect the ionic conductivity and durability of conductivity. Solid-state pulsed-field gradient nuclear magnetic resonance (PFG-NMR)verified the high mobility of H+ and Li+ ions in the temperature range of 300-400 K. In particular, the insertion of Li salts improved the H+ mobility above 373 K owing to strong binding with H2O. Furthermore, the continuous increase in Li+ mobility with temperature contributed to the retention of the overall high ionic conductivity at high temperatures.

Cooperative Proton and Li‐ion Conduction in a 2D‐Layered MOF via Mechanical Insertion of Lithium Halides

AbstractIonic conduction in highly designable and porous metal–organic frameworks has been explored through the introduction of various ionic species (H+, OH−, Li+, etc.) using post‐synthetic modification such as acid, salt, or ionic liquid incorporation. Here, we report on high ionic conductivity (σ>10−2 S cm−1) in a two‐dimensionally (2D)‐layered Ti‐dobdc (Ti2(Hdobdc)2(H2dobdc), H4dobdc: 2,5‐dihydroxyterephthalic acid) via LiX (X=Cl, Br, I) intercalation using mechanical mixing. The anionic species in lithium halide strongly affect the ionic conductivity and durability of conductivity. Solid‐state pulsed‐field gradient nuclear magnetic resonance (PFG NMR ) verified the high mobility of H+ and Li+ ions in the temperature range of 300–400 K. In particular, the insertion of Li salts improved the H+ mobility above 373 K owing to strong binding with H2O. Furthermore, the continuous increase in Li+ mobility with temperature contributed to the retention of the overall high ionic conductivity at high temperatures.

A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High‐Concentration Electrolytes over Electrochemical Performance of Lithium‐Ion Batteries

AbstractLocalized high‐concentration electrolytes (LHCEs) based on five different types of solvents were systematically studied and compared in lithium (Li)‐ion batteries (LIBs). The unique solvation structure of LHCEs promotes the participation of Li salt in forming solid electrolyte interphase (SEI) on graphite (Gr) anode, which enables solvents previously considered incompatible with Gr to achieve reversible lithiation/delithiation. However, the long cyclability of LIBs is still subject to the intrinsic properties of the solvent species in LHCEs. Such issue can be readily resolved by introducing a small amount of additive into LHCEs. The synergetic decompositions of Li salt, solvating solvent and additive yield effective SEIs and cathode electrolyte interphases (CEIs) in most of the studied LHCEs. This study reveals that both the structure and the composition of solvation sheaths in LHCEs have significant effect on SEI and CEI, and consequently, the cycle life of energetically dense LIBs.

A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High-Concentration Electrolytes over Electrochemical Performance of Lithium-Ion Batteries.

Localized high-concentration electrolytes (LHCEs) based on five different types of solvents were systematically studied and compared in lithium (Li)-ion batteries (LIBs). The unique solvation structure of LHCEs promotes the participation of Li salt in forming solid electrolyte interphase (SEI) on graphite (Gr) anode, which enables solvents previously considered incompatible with Gr to achieve reversible lithiation/delithiation. However, the long cyclability of LIBs is still subject to the intrinsic properties of the solvent species in LHCEs. Such issue can be readily resolved by introducing a small amount of additive into LHCEs. The synergetic decompositions of Li salt, solvating solvent and additive yield effective SEIs and cathode electrolyte interphases (CEIs) in most of the studied LHCEs. This study reveals that both the structure and the composition of solvation sheaths in LHCEs have significant effect on SEI and CEI, and consequently, the cycle life of energetically dense LIBs.

Removal of Na and K from aqueous solutions of Li salts

ABSTRACT The sorption properties of manganese (III, IV), the ferrocyanides sorbents to Na+ and K+ in Li salts water solutions have been studied. The sorption properties of the sorbents have been determined under batch and dynamic conditions using Li salts water solutions. The granulated sorbents, based on manganese oxide, obtained via interaction of KMnO4 and H2O2 solution, heated at 500°C, with NaOH or KOH, have the best characteristics. These sorbents are also chemically and mechanically stable for implementing them in the sorption-desorption procedure. The sorption resource of the granulated manganese oxide until the 50% breakthrough of sodium is 60 bed volumes, the potassium is 280 bed volumes. The investigated sorbents can be used in Na+ and K+ ions extraction for obtaining highly purified lithium salts.

A dielectric electrolyte composite with high lithium-ion conductivity for high-voltage solid-state lithium metal batteries.

The ionic conductivity of composite solid-state electrolytes does not meet the application requirements of solid-state lithium (Li) metal batteries owing to the harsh space charge layer of different phases and low concentration of movable Li+. Herein, we propose a robust strategy for creating high-throughput Li+ transport pathways by coupling the ceramic dielectric and electrolyte to overcome the low ionic conductivity challenge of composite solid-state electrolytes. A highly conductive and dielectric composite solid-state electrolyte is constructed by compositing the poly(vinylidene difluoride) matrix and the BaTiO3-Li0.33La0.56TiO3-x nanowires with a side-by-side heterojunction structure (PVBL). The polarized dielectric BaTiO3 greatly promotes the dissociation of Li salt to produce more movable Li+, which locally and spontaneously transfers across the interface to coupled Li0.33La0.56TiO3-x for highly efficient transport. The BaTiO3-Li0.33La0.56TiO3-x effectively restrains the formation of the space charge layer with poly(vinylidene difluoride). These coupling effects contribute to a quite high ionic conductivity (8.2 × 10-4 S cm-1) and lithium transference number (0.57) of the PVBL at 25 °C. The PVBL also homogenizes the interfacial electric field with electrodes. The LiNi0.8Co0.1Mn0.1O2/PVBL/Li solid-state batteries stably cycle 1,500 times at a current density of 180 mA g-1, and pouch batteries also exhibit an excellent electrochemical and safety performance.