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1.
Proc Natl Acad Sci U S A ; 119(41): e2211059119, 2022 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-36191201

RESUMO

All-solid-state Li-metal batteries (ASSLBs) are highly desirable, due to their inherent safety and high energy density; however, the irregular and uncontrolled growth of Li filaments is detrimental to interfacial stability and safety. Herein, we report on the incorporation of piezo-/ferroelectric BaTiO3 (BTO) nanofibers into solid electrolytes and determination of electric-field distribution due to BTO inclusion that effectively regulates the nucleation and growth of Li dendrites. Theoretical simulations predict that the piezoelectric effect of BTO embedded in solid electrolyte reduces the driving force of dendrite growth at high curvatures, while its ferroelectricity reduces the overpotential, which helps to regularize Li deposition and Li+ flux. Polarization reversal of soft solid electrolytes was identified, confirming a regular deposition and morphology alteration of Li. As expected, the ASSLBs operating with LiFePO4/Li and poly(ethylene oxide) (PEO)/garnet solid electrolyte containing 10% BTO additive showed a steady and long cycle life with a reversible capacity of 103.2 mAh g-1 over 500 cycles at 1 C. Furthermore, the comparable cyclability and flexibility of the scalable pouch cells prepared and the successful validation in the sulfide electrolytes, demonstrating its universal and promising application for the integration of Li metal anodes in solid-state batteries.

2.
Small ; 20(14): e2307116, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-37988688

RESUMO

Iron trifluoride (FeF3) is attracting tremendous interest due to its lower cost and the possibility to enable higher energy density in lithium-ion batteries. However, its cycle performance deteriorates rapidly in less than 50 cycles at elevated temperatures due to cracking of the unstable cathode solid electrolyte interface (CEI) followed by active materials dissolution in liquid electrolyte. Herein, by engineering the salt composition, the Fe3O4-type CEI with the doping of boron (B) atoms in a polymer electrolyte at 60 °C is successfully stabilized. The cycle life of the well-designed FeF3-based composite cathode exceeds an unprecedented 1000 cycles and utilizes up to 70% of its theoretical capacities. Advanced electron microscopy combined with density functional theory (DFT) calculations reveal that the B in lithium salt migrates into the cathode and promotes the formation of an elastic and mechanic robust boron-contained CEI (BOR-CEI) during cycling, by which the durability of the CEI to frequent cyclic large volume changes is significantly enhanced. To this end, the notorious active materials dissolution is largely prohibited, resulting in a superior cycle life. The results suggest that engineering the CEI such as tuning its composition is a viable approach to achieving FeF3 cathode-based batteries with enhanced performance.

3.
Small ; : e2401892, 2024 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-38794995

RESUMO

Inorganic solid-state electrolytes have attracted enormous attention due to their potential safety, increased energy density, and long cycle-life benefits. However, their application in solid-state batteries is limited by unstable electrode-electrolyte interface, poor point-to-point physical contact, and low utilization of metallic anodes. Herein, interfacial engineering based on sodium (Na)-conductive polymeric solid-state interfacial adhesive is studied to improve interface stability and optimize physical contacts, constructing a robust organic-rich solid electrolyte interphase layer to prevent dendrite-induced crack propagation and security issues. The interfacial adhesive strategy significantly increases the room-temperature critical current density of inorganic Na-ion conductors from 0.8 to 3.2 mA cm-2 and markedly enhances the cycling performance of solid-state batteries up to 500 cycles, respectively. Particularly, the Na3V2(PO4)3-based full solid-state batteries with high cathode loading of 10.16 mg cm-2 also deliver an excellent cycling performance, further realizing the stable operation of solid-state laminated pouch cells. The research provides fundamental perspectives into the role of interfacial chemistry and takes the field a step closer to realizing practical solid-state batteries.

4.
Small ; 20(24): e2311839, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38155348

RESUMO

Solid-polymer electrolytes comprised of polypropylene carbonate (PPC) and varied sodium bis(fluorosulfonyl)imide (NaFSI) salt concentrations are investigated for implementation as a conductive solid polymer electrolyte into solid-state cathode composites utilizing a sodium-layered oxide active material. The ionic conductivity generally increases with NaFSI salt content, reaching ≈1 mS cm-1 at 80 °C at the highest salt concentration (PPC:NaFSI = 0.5:1). Through an all-in-one slurry casting method, Na2/3Ni1/3Mn2/3O2 cathode composites are fabricated in which the dispersed PPC electrolyte acts as the primary binder. Enabled by a bilayer polymer electrolyte system, cycling performance with the PPC cathode electrolyte is optimized with respect to salt concentration and anode material. The best cyclability is achieved with a moderate salt concentration electrolyte (PPC:NaFSI = 5:1), showcasing an initial capacity of 83 mA h g-1 with a remarkable 80% capacity retention after 150 cycles at C/5 rate and 60 °C. The superior performance of the lower salt concentration electrolyte is attributed to better electrochemical stability, as confirmed by linear sweep voltammetry and online electrochemical mass spectrometry measurements. These results underscore the potential of carbonate-based polymer electrolytes and the importance of balancing electrolyte conductivity and stability in cell design.

5.
Chemistry ; 30(22): e202304252, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38369896

RESUMO

Ta-doped Li7La3Zr2O12 (LLZTO) solid-state electrolytes (SEs) show great promise for solid-state batteries due to its high conductivity and safety. However, one of the challenges it faces is lithium dendrite propagation upon long-term cycling. To address this issue, we propose the incorporation of fumed silica (FS) at the grain boundaries of LLZTO to modify the properties of the garnet pellet, which effectively inhibits the dendrite growth. The introduction of FS has demonstrated several beneficial effects. Firstly, it reduces the migration barrier of lithium ions, which helps prevent dendrite formation and propagation. Additionally, FS reduces the electronic conductivity of the SEs pellet, suppressing the dendrite formation. Moreover, the formed lithium silicates from FS might also be acted as electron inhibitor, thus inhibiting the lithium dendrite growth upon cycling. By investigating the use of FS as a modifier in LLZTO-based electrolytes, our study contributes to advancing dendrite-free solid-state electrolytes and thus the development of high-performance all-solid-state batteries.

6.
Nanotechnology ; 35(47)2024 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-39079542

RESUMO

Li-ion battery is currently considered to be the most proven technology for energy storage systems when it comes to the overall combination of energy, power, cyclability and cost. However, there are continuous expectations for cost reduction in large-scale applications, especially in electric vehicles and grids, alongside growing concerns over safety, availability of natural resources for lithium, and environmental remediation. Therefore, industry and academia have consequently shifted their focus towards 'beyond Li-ion technologies'. In this respect, other non-Li-based alkali-ion/polyvalent-ion batteries, non-Li-based all solid-state batteries, fluoride-ion/ammonium-ion batteries, redox-flow batteries, sand batteries and hydrogen fuel cells etc. are becoming potential cost-effective alternatives. While there has been notable swift advancement across various materials, chemistries, architectures, and applications in this field, a comprehensive overview encompassing high-energy 'beyond Li-ion' technologies, along with considerations of commercial viability, is currently lacking. Therefore, in this review article, a rationalized approach is adopted to identify notable 'post-Li' candidates. Their pros and cons are comprehensively presented by discussing the fundamental principles in terms of material characteristics, relevant chemistries, and architectural developments that make a good high-energy 'beyond Li' storage system. Furthermore, a concise summary outlining the primary challenges of each system is provided, alongside the potential strategies being implemented to mitigate these issues. Additionally, the extent to which these strategies have positively influenced the performance of these 'post-Li' technologies is discussed.

7.
Sensors (Basel) ; 24(8)2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38676011

RESUMO

With the in-depth study of solid-state batteries (SSBs), various in situ and ex situ characterization technologies have been widely used to study them. The performance and reliability of SSBs are limited by the formation and evolution of lithium dendrites at the interfaces between solid electrodes and solid electrolytes. We propose a new method based on optical coherence tomography (OCT) for in situ characterization of the internal state of solid-state batteries. OCT is a low-loss, high-resolution, non-invasive imaging technique that can provide real-time monitoring of cross-sectional images of internal structures of SSBs. The morphology, growth, and evolution of lithium dendrites at different stages of cycling under various conditions can be visualized and quantified by OCT. Furthermore, we validate and correlate the OCT results with scanning electron microscopy (SEM) and XPS, proving the accuracy and effectiveness of the OCT characterization method. We reveal the interfacial phenomena and challenges in SSBs and demonstrate the feasibility and advantages of OCT as a powerful tool for in situ and operando imaging of battery interfaces. This study provides new insights into the mechanisms and factors that affect SSB performance, safety, and lifetime, and suggests possible solutions for improvement and application in the field of applied energy.

8.
Nano Lett ; 23(23): 10856-10863, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-37982531

RESUMO

All-solid-state sulfide-based Li metal batteries are promising candidates for energy storage systems. However, thorny issues associated with undesired reactions and contact failure at the anode interface hinder their commercialization. Herein, an indium foil was endowed with a formed interlayer whose surface film is enriched with LiF and LiIn phases via a feasible prelithiation route. The lithiated alloy of the interlayer can regulate Li+ flux and charge distribution as a Li reservoir, benefiting uniform Li deposition. Meanwhile, it can suppress the reductive decomposition of the Li6PS5Cl electrolyte and maintain sufficient solid-solid contact. In situ impedance spectra reveal that constant interface impedance and fast charge transfer are realized by the interlayer. Further, long-term Li stripping/plating over 2000 h at 2.55 mA cm-2 is demonstrated by this anode. All-solid-state cells employing a LiCoO2 cathode and the Pre In anode can work for over 700 cycles with a capacity retention of 96.15% at 0.5 C.

9.
Angew Chem Int Ed Engl ; 63(19): e202402274, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38415322

RESUMO

The high theoretical energy density (1274 Wh kg-1) and high safety enable the all-solid-state Na-S batteries with great promise for stationary energy storage system. However, the uncontrollable solid-liquid-solid multiphase conversion and its associated sluggish polysulfides redox kinetics pose a great challenge in tunning the sulfur speciation pathway for practical Na-S electrochemistry. Herein, we propose a new design methodology for matrix featuring separated bi-catalytic sites that control the multi-step polysulfide transformation in tandem and direct quasi-solid reversible sulfur conversion during battery cycling. It is revealed that the N, P heteroatom hotspots are more favorable for catalyzing the long-chain polysulfides reduction, while PtNi nanocrystals manipulate the direct and full Na2S4 to Na2S low-kinetic conversion during discharging. The electrodeposited Na2S on strongly coupled PtNi and N, P-codoped carbon host is extremely electroreactive and can be readily recovered back to S8 without passivation of active species during battery recharging, which delivers a true tandem electrocatalytic quasi-solid sulfur conversion mechanism. Accordingly, stable cycling of the all-solid-state soft-package Na-S pouch cells with an attractive specific capacity of 876 mAh gS -1 and a high energy of 608 Wh kgcathode -1 (172 Wh kg-1, based on the total mass of cathode and anode) at 60 °C are demonstrated.

10.
Angew Chem Int Ed Engl ; : e202410463, 2024 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-39141694

RESUMO

Solid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces Ga62.5In21.5Sn16 (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self-healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li-ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li-LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid-state Li/LiFePO4 battery achieves promising full-cell functionality with notable rate performance and stable cycle life. This active filler-mediated self-healing approach could bring new insights into the battery design in versatile solid-state systems.

11.
Angew Chem Int Ed Engl ; : e202416170, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39235148

RESUMO

Solid polymer electrolytes (SPEs) are crucial in the development of lithium metal batteries. Recently, metal-organic frameworks (MOFs) with open metal sites (OMSs) have shown promise as solid fillers to improve the performance of SPEs. However, the number of OMS-containing MOFs is quite limited, comprising less than 5% of the total MOFs. When considering yield, cost, and processability, the commonly used OMS-containing MOFs are no more than 10 types, causing great limitations. Herein, we reported a simple and universal methodology that converted OMS-free MOFs to OMS-rich quasi-MOFs for developing high-performance SPEs, and explored the underlying mechanism. The "OMS-polymer" and "OMS-ion" interactions were investigated in detail to elucidate the role of quasi-MOFs on battery performance. It was found that quasi-MOFs, functioning as ion sieves, can effectively regulate ion migration, thus promoting uniform Li deposition and enabling an ultra-stable interface. As a result, the Li symmetric cell stably ran over 3000 h at 0.3 mA cm-2, while the full cell retained 85% of its initial capacity after 1500 cycles at 1.0 C. Finally, universal testing was performed using other MOFs, confirming the generalizability and effectiveness of our design concept.

12.
Angew Chem Int Ed Engl ; 63(1): e202315856, 2024 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-37985233

RESUMO

Solid-state batteries (SSBs) based on Li-rich Mn-based oxide (LRMO) cathodes attract much attention because of their high energy density as well as high safety. But their development was seriously hindered by the interfacial instability and inferior electrochemical performance. Herein, we design a three-dimensional foam-structured GaN-Li composite anode and successfully construct a high-performance SSB based on Co-free Li1.2 Ni0.2 Mn0.6 O2 cathode and Li6.5 La3 Zr1.5 Ta0.5 O12 (LLZTO) solid electrolyte. The interfacial resistance is considerably reduced to only 1.53â€…Ω cm2 and the assembled Li symmetric cell is stably cycled more than 10,000 h at 0.1-0.2 mA cm-2 . The full battery shows a high initial capacity of 245 mAh g-1 at 0.1 C and does not show any capacity degradation after 200 cycles at 0.2 C (≈100 %). The voltage decay is well suppressed and it is significantly decreased from 2.96 mV/cycle to only 0.66 mV/cycle. The SSB also shows a very high rate capability (≈170 mAh g-1 at 1 C) comparable to a liquid electrolyte-based battery. Moreover, the oxygen anion redox (OAR) reversibility of LRMO in SSB is much higher than that in liquid electrolyte-based cells. This study offers a distinct strategy for constructing high-performance LRMO-based SSBs and sheds light on the development and application of high-energy density SSBs.

13.
Angew Chem Int Ed Engl ; : e202413502, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39136325

RESUMO

Garnet Li7La3Zr2O12 (LLZO)-based solid-state electrolytes (SSEs) hold promise for realizing next-generation lithium metal batteries with high energy density. However, the high stiffness of high-temperature sintered LLZO makes it brittle and susceptible to strain during the fabrication of solid-state batteries. Cold-pressed LLZO exhibits improved ductility but suffers from insufficient Li+ conductivity. Here, we report cold-pressed Ta-doped LLZO (Ta-LZ) particles integrated with ductile Li6PS5Cl (LPSC) via a Li+ conductive Li-containing Ta-Cl structure. This configuration creates a continuous Li+ conduction network by enhancing the Li+ exchange at the Ta-LZ/LPSC interface. The resulting Ta-LZ/LPSC SSE exhibits Li+ conductivity of 4.42 × 10-4 S cm-1 and a low activation energy of 0.31 eV. Li symmetric cells with Ta-LZ/LPSC SSE demonstrate excellent Li dendrite suppression ability, with an improved critical current density of 5.0 mA cm-2 and a prolonged cycle life exceeding 600 h at 1 mA cm-2. Our finding provides valuable insights into developing cold-pressed ceramic powder electrolytes for high-performance all-solid-state batteries.

14.
Angew Chem Int Ed Engl ; 63(33): e202403617, 2024 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-38819860

RESUMO

All-solid-state lithium batteries (ASSBs) have received increasing attentions as one promising candidate for the next-generation energy storage devices. Among various solid electrolytes, sulfide-based ASSBs combined with layered oxide cathodes have emerged due to the high energy density and safety performance, even at high-voltage conditions. However, the interface compatibility issues remain to be solved at the interface between the oxide cathode and sulfide electrolyte. To circumvent this issue, we propose a simple but effective approach to magic the adverse surface alkali into a uniform oxyhalide coating on LiNi0.8Co0.1Mn0.1O2 (NCM811) via a controllable gas-solid reaction. Due to the enhancement of the close contact at interface, the ASSBs exhibit improved kinetic performance across a broad temperature range, especially at the freezing point. Besides, owing to the high-voltage tolerance of the protective layer, ASSBs demonstrate excellent cyclic stability under high cutoff voltages (500 cycles~94.0 % at 4.5 V, 200 cycles~80.4 % at 4.8 V). This work provides insights into using a high voltage stable oxyhalide coating strategy to enhance the development of high energy density ASSBs.

15.
Angew Chem Int Ed Engl ; 63(27): e202401373, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38659181

RESUMO

Inorganic solid-state electrolytes (SSEs) play a vital role in high-energy all-solid-state batteries (ASSBs). However, the current method of SSE preparation usually involves high-energy mechanical ball milling and/or a high-temperature annealing process, which is not suitable for practical application. Here, a facile strategy is developed to realize the scalable synthesis of cost-effective aluminum-based oxyhalide SSEs, which involves a self-propagating method by the exothermic reaction of the raw materials. This strategy enables the synthesis of various aluminum-based oxyhalide SSEs with tunable components and high ionic conductivities (over 10-3 S cm-1 at 25 °C) for different cations (Li+, Na+, Ag+). It is elucidated that the amorphous matrix, which mainly consists of various oxidized chloroaluminate species that provide numerous sites for smooth ion migration, is actually the key factor for the achieved high conductivities. Benefit from their easy synthesis, low cost, and low weight, the aluminum-based oxyhalide SSEs synthesized by our approach could further promote practical application of high-energy-density ASSBs.

16.
Angew Chem Int Ed Engl ; 63(6): e202317776, 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38117014

RESUMO

The broader implementation of current all-solid-state Na-S batteries is still plagued by high operation temperature and inefficient sulfur utilization. And the uncontrollable sulfur speciation pathway along with the sluggish polysulfide redox kinetics further compromise the theoretical potentials of Na-S chemistry. Herein, we report a confined bidirectional tandem electrocatalysis effect to tune polysulfide electrochemistry in a novel low-temperature (80 °C) all-solid-state Na-S battery that utilizes Na3 Zr2 Si2 PO12 ceramic membrane as a platform. The bifunctional hollow sulfur matrix consisting binary atomically dispersed MnN4 and CoN4 hotspots was fabricated using a sacrificial template process. Upon discharge, CoN4 sites activate sulfur species and catalyze long-chain to short-chain polysulfides reduction, while MnN4 centers substantially accelerate the low-kinetic Na2 S4 to Na2 S directly conversion, manipulating the uniform deposition of electroactive Na2 S and avoiding the formation of irreversible products (e.g., Na2 S2 ). The intrinsic synergy of two catalytic centers benefits the Na2 S decomposition and minimizes its activation barrier during battery recharging and then efficiently mitigate the cathodic passivation. As a result, the stable cycling of all-solid-state Na-S cell delivers an attractive reversible capacity of 1060 mAh g-1 with a high CE of 98.5 % and a high energy of 1008 Wh kgcathode -1 , comparable to the liquid electrolyte cells.

17.
Nanotechnology ; 34(15)2023 Feb 03.
Artigo em Inglês | MEDLINE | ID: mdl-36649649

RESUMO

Battery safety calls for solid state batteries and how to prepare solid electrolytes with excellent performance are of significant importance. In this study, hybrid solid electrolytes combined with organic PVDF-HFP and inorganic active fillers are studied. The modified active fillers of Li7-x-3yAlyLa3Zr2-xTaxO12are obtained by co-element doping with Al and Ta when LLZO is synthesized by calcination. And an high room temperature ionic conductivity of 5.357 × 10-4S cm-1is exhibited by ATLLZO ceramic sheet. The composite solid electrolyte PVDF-HFP/LiTFSI/ATLLZO (PHL-ATLLZO) is prepared by solution casting method, and its electrochemical properties are investigated. The results show that when the contents of lithium salt LiTFSI and active filler ATLLZO are controlled at 40 wt% and 10%, respectively, the ionic conductivity of the resulting composite solid electrolyte is as high as 2.686 × 10-4S cm-1at room temperature, and a wide electrochemical window of 4.75 V is exhibited. The LiFePO4/PHL-ATLLZO/Li all-solid-state battery assembled based on the composite solid-state electrolyte exhibits excellent cycling stability at room temperature. The cell assembled by casting the composite solid-state electrolyte on the cathode surface shows a discharge specific capacity of 134.3 mAh g-1and 96.2% capacity retention after 100 cycles at 0.2 C. The prepared composite solid-state electrolyte demonstrates excellent electrochemical performance.

18.
Nano Lett ; 22(12): 4905-4911, 2022 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-35687074

RESUMO

Structural evolutions are crucial for determining the performance of high-voltage lithium, manganese-rich layered cathodes. Moreover, interface between electrode and electrolyte plays a critical role in governing ionic transfer in all-solid-state batteries. Here, we unveil two different types of porous structure in Li1.2Ni0.2Mn0.6O2 cathode with LiPON solid-state electrolyte. Nanopores are found near the cathode/electrolyte interface at pristine state, where cation mixing, phase transformation, oxygen loss, and Mn reduction are also found. In situ Li+ extraction induces the evolution of nanovoids, initially formed near the interface then propagated into the bulk. Despite the development of nanovoids, layered structure is conserved, suggesting the nature of nanopores and nanovoids are different and their impact would be divergent. This work demonstrates the intrinsic interfacial layer, as well as the dynamic scenario of nanovoid formation inside high-capacity layered cathode, which helps to understand the performance fading in cathodes and offers insight into the all-solid-state battery design.

19.
Nano Lett ; 22(20): 8346-8354, 2022 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-36219091

RESUMO

Sulfide electrolytes promise superior ion conduction in all-solid-state lithium (Li) metal batteries, while suffering harsh hurdles including interior dendrite growth and instability against Li and moist air. A prerequisite for solving such issues is to uncover the nature of the Li/sulfide interface. Herein, air-stable Li4SnS4 (LSS) as a prototypical sulfide electrolyte is selected to visualize the dynamic evolution and failure of the Li/sulfide interface by cryo-electron microscopy. The interfacial parasitic reaction (2Li + 2Li4SnS4 = 5Li2S + Sn2S3) is validated by direct detection of randomly distributed Li2S and Sn2S3 crystals. A bifunctional buffering layer is consequently introduced by self-diffusion of halide into LSS. Both the interface and the grain boundaries in LSS have been stabilized, eliminating the growing path of Li dendrites. The buffering layer enables the durability of Li symmetric cell (1500 h) and high-capacity retention of the LiFePO4 full-cell (95%). This work provides new insights into the hierarchical design of sulfide electrolytes.

20.
Molecules ; 28(8)2023 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-37110777

RESUMO

Due to the limitations of organic liquid electrolytes, current development is towards high performance all-solid-state lithium batteries (ASSLBs). For high performance ASSLBs, the most crucial is the high ion-conducting solid electrolyte (SE), with a focus on interface analysis between SE and active materials. In the current study, we successfully synthesized the high ion-conductive argyrodite-type (Li6PS5Cl) solid electrolyte, which has 4.8 mS cm-1 conductivity at room temperature. Additionally, the present study suggests the quantitative analysis of interfaces in ASSLBs. The measured initial discharge capacity of a single particle confined in a microcavity electrode was 1.05 nAh for LiNi0.6Co0.2Mn0.2O2 (NCM622)-Li6PS5Cl solid electrolyte materials. The initial cycle result shows the irreversible nature of active material due to the formation of the solid electrolyte interphase (SEI) layer on the surface of the active particle; further second and third cycles demonstrate high reversibility and good stability. Furthermore, the electrochemical kinetic parameters were calculated through the Tafel plot analysis. From the Tafel plot, it is seen that asymmetry increases gradually at high discharge currents and depths, which rise asymmetricity due to the increasing of the conduction barrier. However, the electrochemical parameters confirm the increasing conduction barrier with increased charge transfer resistance.

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