Constructing Nano-Interlayer Inhibiting Interfacial Degradation toward High-Voltage PEO-Based All-Solid-State Lithium Batteries.

The interfacial instability between PEO-based solid electrolyte (SPE) and high-voltage cathode materials inhibits the longevity of high-energy-density all-solid-state polymer lithium metal batteries (ASSPLBs). Herein, for the first time it is demonstrated, that contact loss caused by gas generation from interfacial side reactions between the high-voltage cathode and solid polymer electrolyte (SPE) can also arise in ASSPLBs. To alleviate the interfacial side reactions, a LiNb0.6Ti0.5O3 (LNTO) layer is well coated on LiNi0.83Co0.07Mn0.1O2 (NCM83), denoted as (CNCM83). The LNTO layer with low electronic conductivity reduces the decomposition drive force of SPE. Furthermore, Ti and Nb in the LNTO layer spontaneously migrate inside the NCM83 surface to form a strong Ti/Nb─O bond, stalling oxygen evolution in high-voltage cathodes. The interfacial degradation phenomena, including SPE decomposition, detrimental phase transition and intragranular cracks of NCM83, and void formation between cathode and SPE, are effectively mitigated by the LNTO layer. Therefore, the growth rate of interfacial resistance (RCEI) decreases from 37.6 Ω h-0.5 for bare NCM83 to 2.4 Ω h-0.5 for CNCM83 at 4.2 V. Moreover, 4.2 V PEO-based ASSPLBs achieve impressive cyclability with high capacity retention of 135 mAh g-1 (75%) even after 300 cycles at 0.5 C.

Biophysical Modelling for Insight into Oxygen Diffusion, Distribution, and Measurement.

Building on an extensive history of physiological and systems-oriented modelling, my group and others have recently used molecular simulation studies to understand oxygen (O2) transport and localisation. Molecular simulations enable biophysical insight into processes difficult to study with experiments alone and are sometimes described as a "computational microscope." Our work has emphasised lipid membrane contributions to oxygen diffusion and uptake, suggesting that lipid-based pathways along membranes and lipid deposits are likely to accelerate diffusive transport through cells and tissues. Moreover, the lipid and fluid fractions of the tissue are expected to be primary determinants of the local oxygen partial pressure (pO2) as well as the oxygen permeability. Measurements using molecular probes can be influenced by the local molecular environment, due to differential solubility of both the probe and the oxygen molecules in various components of the cell's complex solvent system. The biomolecular simulation work complements experimental studies, which enable evaluation of the models' accuracy and their applicability to real biological systems. Further work is needed to assess fully the possible influence of nanoscale crowders and obstacles (especially protein molecules) on tissue-level diffusive transport of oxygen. Likewise, water-rich carbohydrate layers, such as the glycocalyx, should be evaluated as potential barriers to oxygen transport. Insights gained through biophysical modelling studies could be broadly relevant to clinical phenomena affected by tissue oxygenation, such as tumour radiotherapy, ischaemia, neuropathy, and wound healing.

Supramolecular Polymer Ion Conductor with Weakened Li Ion Solvation Enables Room Temperature All-Solid-State Lithium Metal Batteries.

Improved durability, enhanced interfacial stability, and room temperature applicability are desirable properties for all-solid-state lithium metal batteries (ASSLMBs), yet these desired properties are rarely achieved simultaneously. Here, in this work, it is noticed that the huge resistance at Li metal/electrolyte interface dominantly impeded the normal cycling of ASSLMBs especially at around room temperature (<30 °C). Accordingly, a supramolecular polymer ion conductor (SPC) with "weak solvation" of Li+ was prepared. Benefiting from the halogen-bonding interaction between the electron-deficient iodine atom (on 1,4-diiodotetrafluorobenzene) and electron-rich oxygen atoms (on ethylene oxide), the O-Li+ coordination was significantly weakened. Therefore, the SPC achieves rapid Li+ transport with high Li+ transference number, and importantly, derives a unique Li2 O-rich SEI with low interfacial resistance on lithium metal surface, therefore enabling stable cycling of ASSLMBs even down to 10 °C. This work is a new exploration of halogen-bonding chemistry in solid polymer electrolyte and highlights the importance of "weak solvation" of Li+ in the solid-state electrolyte for room temperature ASSLMBs.

Quantitative Analyses of the Interfacial Properties of Current Collectors at the Mesoscopic Level in Lithium Ion Batteries by Using Hierarchical Graphene.

At the mesoscopic level of commercial lithium ion battery (LIB), it is widely believed that the poor contacts between current collector (CC) and electrode materials (EM) lead to weak adhesions and large interfacial electric resistances. However, systematic quantitative analyses of the influence of the interfacial properties of CC are still scarce. Here, we built a model interface between CC and electrode materials by directly growing hierarchical graphene films on commercial Al foil CC, and we performed systematic quantitative studies of the interfacial properties therein. Our results show that the interfacial electric resistance dominates, i.e. ∼2 orders of magnitude higher than that of electrode materials. The interfacial resistance could be eliminated by hierarchical graphene interlayer. Cathode on CC with eliminated interfacial resistance could deliver much improved power density outputs. Our work quantifies the mesoscopic factors influencing the battery performance and offers practical guidelines of boosting the performance of LIBs and beyond.

Li3N-Modified Garnet Electrolyte for All-Solid-State Lithium Metal Batteries Operated at 40 °C.

Lithium carbonate on the surface of garnet blocks Li+ conduction and causes a huge interfacial resistance between the garnet and electrode. To solve this problem, this study presents an effective strategy to reduce significantly the interfacial resistance by replacing Li2CO3 with Li ion conducting Li3N. Compared to the surface Li2CO3 on garnet, Li3N is not only a good Li+ conductor but also offers a good wettability with both the garnet surface and a lithium metal anode. In addition, the introduction of a Li3N layer not only enables a stable contact between the Li anode and garnet electrolyte but also prevents the direct reduction of garnet by Li metal over a long cycle life. As a result, a symmetric lithium cell with this Li3N-modified garnet exhibits an ultralow overpotential and stable plating/stripping cyclability without lithium dendrite growth at room temperature. Moreover, an all-solid-state Li/LiFePO4 battery with a Li3N-modified garnet also displays high cycling efficiency and stability over 300 cycles even at a temperature of 40 °C.

Electrochemical Properties of Nitrate-Selective Electrodes: The Dependence of Resistance on the Solution Concentration.

The electrochemical properties of ion-exchanger-based solvent polymeric ion-selective electrodes (ISEs)—bulk and interfacial resistance, capacitance, and polarization under a galvanostatic current step—are studied, with a nitrate ISE based on tetradecylammonium nitrate (TDANO3) as a model system. The study is performed by chronopotentiometric and impedance measurements, and focuses on the dependence of the aforementioned properties on the concentration of NO3− anions in solution. The impacts from the bulk and the interfacial charge transfer to the overall membrane resistance are revealed. It is shown that the bulk resistance of the membranes decreases over an increase of NO3− concentration within the range of a Nernstian potentiometric response of the ISE. This fact, also reported earlier for K⁺- and Ca2+-selective ISEs, is not in line with current views of the mechanism of the ISE response, or of the role of ion exchange in particular. The origin of this effect is unclear. Estimates are made for the concentration of ionized species (NO3− and TDA⁺) and, respectively, for the TDANO3 association constant, as well as for the species diffusion coefficients in the membrane.

Manipulating the Flow of Nanoconfined Water by Temperature Stimulation.

The manipulation of a nanoconfined fluid flow is a great challenge and is critical in both fundamental research and practical applications. Compared with chemical or biochemical stimulation, the use of temperature as controllable, physical stimulation possesses huge advantages, such as low cost, easy operation, reversibility, and no contamination. We demonstrate an elegant, simple strategy by which temperature stimulation can readily manipulate the nanoconfined water flow by tuning interfacial and viscous resistances. We show that with an increase in temperature, the water fluidity is decreased in hydrophilic nanopores, whereas it is enhanced by at least four orders of magnitude in hydrophobic nanopores, especially in carbon nanotubes with a controlled size and atomically smooth walls. We attribute these opposing trends to a dramatic difference in varying surface wettability that results from a small temperature variation.

A Perovskite Electrolyte That Is Stable in Moist Air for Lithium-Ion Batteries.

Solid-oxide Li+ electrolytes of a rechargeable cell are generally sensitive to moisture in the air as H+ exchanges for the mobile Li+ of the electrolyte and forms insulating surface phases at the electrolyte interfaces and in the grain boundaries of a polycrystalline membrane. These surface phases dominate the total interfacial resistance of a conventional rechargeable cell with a solid-electrolyte separator. We report a new perovskite Li+ solid electrolyte, Li0.38 Sr0.44 Ta0.7 Hf0.3 O2.95 F0.05 , with a lithium-ion conductivity of σLi =4.8×10-4  S cm-1 at 25 °C that does not react with water having 3≤pH≤14. The solid electrolyte with a thin Li+ -conducting polymer on its surface to prevent reduction of Ta5+ is wet by metallic lithium and provides low-impedance dendrite-free plating/stripping of a lithium anode. It is also stable upon contact with a composite polymer cathode. With this solid electrolyte, we demonstrate excellent cycling performance of an all-solid-state Li/LiFePO4 cell, a Li-S cell with a polymer-gel cathode, and a supercapacitor.

Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries.

Li7 La3 Zr2 O12 -based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li2 CO3 layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. Here, we introduce LiF to garnet Li6.5 La3 Zr1.5 Ta0.5 O12 (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li2 CO3 on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. An all-solid-state Li/polymer/LLZT-2LiF/LiFePO4 battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.

Piezoelectric Interlayer Enabling a Rechargeable Quasisolid-State Sodium Battery at 0 °C.

Solid-state sodium (Na) batteries (SSNBs) hold great promise but suffer from several major issues, such as high interfacial resistance at the solid electrolyte/electrode interface and Na metal dendrite growth. To address these issues, a piezoelectric interlayer design for an Na3Zr2Si2PO12 (NZSP) solid electrolyte is proposed herein. Two typical piezoelectric films, AlN and ZnO, coated onto NZSP function as interlayers designed to generate a local stress-induced field for alleviating interfacial charge aggregation coupling stress concentration and promoting uniform Na plating. The results reveal that the interlayer (ZnO) with matched modulus, high Na-adhesion, and sufficient piezoelectricity can provide a favorable interphase. Low interfacial resistances of 91 and 239 Ω cm2 are achieved for the ZnO layer at 30 and 0 °C, respectively, which are notably lower than those for bare NZSP. Moreover, steady Na plating/stripping cycles are rendered over 850 and 4900 h at 0 and 30 °C, respectively. The superior anodic performance is further manifested in an Na2MnFe(CN)6-based full cell which delivers discharge capacities of 125 mA h g-1 over 1600 cycles at 30 °C and 90 mA h g-1 over 500 cycles at 0 °C. A new interlayer-design insight is clearly demonstrated for SSNBs breaking low-temperature limits.

What Exactly Can Bionic Strategies Achieve for Flexible Sensors?

Flexible sensors have attracted great attention in the field of wearable electronic devices due to their deformability, lightness, and versatility. However, property improvement remains a key challenge. Fortunately, natural organisms exhibit many unique response mechanisms to various stimuli, and the corresponding structures and compositions provide advanced design ideas for the development of flexible sensors. Therefore, this Review highlights recent advances in sensing performance and functional characteristics of flexible sensors from the perspective of bionics for the first time. First, the "twins" of bionics and flexible sensors are introduced. Second, the enhancements in electrical and mechanical performance through bionic strategies are summarized according to the prototypes of humans, plants, and animals. Third, the functional characteristics of bionic strategies for flexible sensors are discussed in detail, including self-healing, color-changing, tangential force, strain redistribution, and interfacial resistance. Finally, we summarize the challenges and development trends of bioinspired flexible sensors. This Review aims to deepen the understanding of bionic strategies and provide innovative ideas and references for the design and manufacture of next-generation flexible sensors.

State of Charge-Dependent Impedance Spectroscopy as a Helpful Tool to Identify Reasons for Fast Capacity Fading in All-Solid-State Batteries.

Thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising candidate for the next generation of energy storage systems. However, thiophosphate-based ASSBs suffer from fast capacity fading with nickel-rich cathode materials. In many reports, this capacity fading is attributed to an increase of the charge transfer resistance of the composite cathode caused by interface degradation and/or chemo-mechanical failure. The change in the charge transfer resistance is typically determined using impedance spectroscopy after charging the cells. In this work, we demonstrate that large differences in the long-term cycling performance also arise in cells, which exhibit a comparable charge transfer resistance at the cathode side. Our results confirm that the charge transfer resistance of the cathode is not necessarily responsible for capacity fading. Other processes, such as resistive processes on the anode side, can also play a major role. Since these processes usually depend on the state of charge, they may not appear in the impedance spectra of fully charged cells; i.e., analyzing the impedance spectra of charged cells alone is insufficient for the identification of major resistive processes. Thus, we recommend measuring the impedance at different potentials to get a complete understanding of the reasons for capacity fading in ASSBs.

Bonding Lithium Metal with Garnet Electrolyte by Interfacial Lithiophobicity/Lithiophilicity Transition Mechanism over 380 °C.

Garnet electrolytes, possessing high ionic conductivity (10-4 -10-3 S cm-1 at room temperature) and excellent chemical/electrochemical compatibility with lithium metal, are expected to be used in solid-state lithium metal batteries. However, the poor solid-solid interfacial contact between lithium and garnet leads to high interfacial resistance, reducing the battery power capability and cyclability. Garnet electrolytes are commonly believed to be intrinsically lithiophilic, and lithiophobic Li2 CO3 on the garnet surface accounted for the poor interfacial contact. Here, it is proposed that the interfacial lithiophobicity/lithiophilicity of garnets (LLZO, LLZTO) can be transformed above a temperature of ≈380 °C. This transition mechanism is also suitable for other materials such as Li2 CO3 , Li2 O, stainless steel, and Al2 O3 . By using this transition mechanism, uniform and even lithium can be strongly bonded no-surface-treated garnet electrolytes with various shapes. The Li-LLZTO interfacial resistance can be reduced to ≈3.6 Ω cm2 and sustainably withstood lithium extraction and insertion for up to 2000 h at 100 µA cm-2 . This high-temperature lithiophobicity/lithiophilicity transition mechanism can help improve the understanding of lithium-garnet interfaces and build practical lithium-garnet solid-solid interfaces.

Rechargeable Solid-State Na-Metal Battery Operating at -20 °C.

Achieving satisfactory performance for a solid-state Na-metal battery (SSNMB) with an inorganic solid electrolyte (SE), especially under freezing temperatures, poses a challenge for stabilizing a Na-metal anode. Herein, this challenge is addressed by utilizing a Natrium super ionic conductor (NASICON) NASICON-type solid electrolyte, enabling the operation of a rechargeable SSNMB over a wide temperature range from -20 to 45 °C. The interfacial resistance at the Na metal/SE interface is only 0.4 Ω cm2 at 45 °C and remains below 110 Ω cm2 even at -20 °C. Remarkably, long-term Na-metal plating/stripping cycles lasting over 2000 h at -20 °C are achieved with minimal polarization voltages at 0.1 mA cm-2 . Further analysis reveals the formation of a uniform Na3- x Cax PO4 interphase layer at the interface, which significantly contributes to the exceptional interfacial performance observed. By employing a Na3 V1.5 Al0.5 (PO4 )3 cathode, the full battery system demonstrates excellent adaptability to low temperatures, exhibiting a capacity of 80 mA h g-1 at -20 °C over 50 cycles and retaining a capacity of 108 mAh g-1 (88.5% of the capacity at 45 °C) at 0 °C over 275 cycles. This research significantly reduces the temperature threshold for SSNMB operation and paves the way toward solid-state batteries suitable for all-season applications.

Enhancing Fast-Charge Capabilities in Solid-State Lithium Batteries through the Integration of High Li0.5La0.5TiO3 (LLTO) Content in the Lithium-Metal Anode.

Solid-state batteries (SSBs), which have high energy density and are safe, are recognized as an important field of study. However, the poor interfacial contact with high resistance, the dendrite problem, and the volume change of the metallic lithium anode prevent the use of SSBs. Li0.5La0.5TiO3 (LLTO) particles and molten lithium were used to create a high-performance LLTO-Li composite lithium with a sequential ion-conducting phase. With garnet electrolytes, this lithium has better wettability and reduced surface tension. To compensate for the lithium depletion that occurs during stripping, the Li-Ti phase with a high ionic diffusion coefficient that forms in the anode can rapidly transport lithium from the bulk to the solid-state interface, ensuring tight interface contact, preventing the formation of gaps, and homogenizing the current and Li+ flux. The LLTO-Li| LLZTO| LLTO-Li symmetric cell exhibits a good cyclic stability of 1000 h at room temperature, a low interfacial resistance of 22 Ω cm2, and a high critical current density of 1.2 mA cm-2. Furthermore, fully built cells with a LiFePO4 cathode showed outstanding cycling performance, maintaining 95% of their capacity after 900 cycles at 1 C and 92% capacity retention after 100 cycles at 2 C.

Elucidating Ion Transport Phenomena in Sulfide/Polymer Composite Electrolytes for Practical Solid-State Batteries.

Despite the enormous interest in inorganic/polymer composite solid-state electrolytes (CSEs) for solid-state batteries (SSBs), the underlying ion transport phenomena in CSEs have not yet been elucidated. Here, we address this issue by formulating a mechanistic understanding of bi-percolating ion channels formation and ion conduction across inorganic-polymer electrolyte interfaces in CSEs. A model CSE is composed of argyrodite-type Li6PS5Cl (LPSCl) and gel polymer electrolyte (GPE, including Li+-glyme complex as an ion-conducting medium). The percolation threshold of the LPSCl phase in the CSE strongly depends on the elasticity of the GPE phase. Additionally, manipulating the solvation/desolvation behavior of the Li+-glyme complex in the GPE facilitates ion conduction across the LPSCl-GPE interface. The resulting scalable CSE (area = 8 × 6 (cm × cm), thickness ~ 40 µm) can be assembled with a high-mass-loading LiNi0.7Co0.15Mn0.15O2 cathode (areal-mass-loading = 39 mg cm-2) and a graphite anode (negative (N)/positive (P) capacity ratio = 1.1) in order to fabricate an SSB full cell with bi-cell configuration. Under this constrained cell condition, the SSB full cell exhibits high volumetric energy density (480 Wh Lcell-1) and stable cyclability at 25 °C, far exceeding the values reported by previous CSE-based SSBs.

Low Interfacial Resistance and Superior Suppression to Li-Dendrite Penetration Facilitated by Air-Stable and Mechanically Robust Al/Mg-Co-Doped Li-La-Zirconate as Electrolyte for Li-Based Solid-State Cells.

In the context of usage as a solid electrolyte (SE) for Li-based solid-state cells, the interfacial characteristics of Li-La-zirconate (LLZO) with the electrodes and the mechanical properties of LLZO influence the overall impedance and stability. In this regard, the newly developed air-stable Al/Mg-co-doped LLZO has been found to possess greater resistance to crack propagation (by ∼31%) and fracture stress (by ∼52%), along with elevated hardness and stiffness, as compared to simply Al-doped LLZO. Furthermore, as directly visualized via cross-section electron microscopy at the Li/LLZO interfaces, the air-stability, along with mechanical robustness of Al/Mg-co-doped LLZO, facilitates the complete absence of impurity phase and cracks at the Li/LLZO interface, unlike for the simply Al-doped LLZO. These result in a very low area specific resistance for the Li/"Al/Mg-co-doped LLZO" interface of ∼9 Ω cm2, which is ∼3 times lower than that at the Li/"Al-doped LLZO" interface and is also among the lowest reported to date for Li/LLZO interfaces, that too sans any surface/interfacial coating/engineering. Galvanostatic Li-plating/stripping cycles indicate that the critical current density toward initiating Li-dendrite nucleation/propagation is higher in the case of Al/Mg-co-doped LLZO SE, viz., ∼0.45 mA/cm2, than for the Al-doped counterpart (viz., ∼0.25 mA/cm2). Furthermore, Li-stripping/plating cycles @ 0.1 mA/cm2 have revealed outstanding stability of polarization voltage up to at least 100 cycles upon using Al/Mg-codoped LLZO as the SE, in contrast to the instability right from the 36th cycle onward with the Al-doped LLZO. This indicates superior suppression toward Li-dendrite nucleation/propagation by the Al/Mg-codoped LLZO, unlike by Al-doped LLZO, as also directly visualized via cross-section electron microscopy post-cycling. The air-stability induced a clean Li/LLZO interface (viz., good contact), which, together with the mechanical robustness of Al/Mg-codoped LLZO, resulted in the very low interfacial resistance and excellent suppression toward Li-dendrite nucleation/propagation, leading to high CCD and very stable long-term Li-stripping/plating. Overall, in addition to highlighting the notable advantages offered by the Al/Mg-co-doped LLZO solid electrolyte, the insights obtained as part of this work are expected to lead to the successful and facile development of high-performance solid-state Li-based cells.

Construction and Interfacial Modification of a ß-PbSnF4 Electrolyte with High Intrinsic Ionic Conductivity for a Room-Temperature Fluoride-Ion Battery.

Solid-state fluoride-ion batteries (FIBs) attract significant attention worldwide because of their high theoretical volume, energy density, and high safety. However, the large interfacial resistance caused by the point-point contact between the electrolyte and the electrode seriously impedes their further development. Using liquid-phase therapy to construct a conformal interface is a good choice to eliminate the influence of inadequate contact between the electrode and the electrolyte. In this study, a ß-PbSnF4 solid-state electrolyte with high room-temperature ionic conductivity is prepared, and a trace amount of the liquid electrolyte (LE) between the electrode and the electrolyte is introduced in order to minimize the interfacial resistance and enhance the cycle life. The Allen-Hickling simulations show that the introduction of an interfacial wetting agent (LE) can significantly reduce the energy barrier of charge transfer and mass transfer processes at the interface and reciprocate FIBs an enhanced interfacial reaction kinetics. As a result, the initial discharge capacity of the fabricated FIBs is 210.5 mAh g-1 and the capacity retention rate is 82.6% after 50 cycles at room temperature, while the initial discharge capacity of the unmodified battery is only 170.9 mAh g-1 and the capacity retention rate is 22.1% after 50 cycles. Therefore, interfacial modification with a trace amount of LE provides a significant exploration for the improvement of FIB performances.

Tuning the Covalent Coupling Degree between the Cathode and Electrolyte for Optimized Interfacial Resistance in Solid-State Lithium Batteries.

The development of promising solid-state lithium batteries has been a challenging task mainly due to the poor interfacial contact and high interfacial resistance at the electrode/solid-state electrolyte (SSE) interface. Herein, we propose a strategy for introducing a class of covalent interactions with varying covalent coupling degrees at the cathode/SSE interface. This method significantly reduces interfacial impedances by strengthening the interactions between the cathode and SSE. By adjusting the covalent coupling degree from low to high, an optimal interfacial impedance of 33 Ω cm-2 was achieved, which is even lower than the interfacial impedance using liquid electrolytes (39 Ω cm-2). This work offers a fresh perspective on solving the interfacial contact problem in solid-state lithium batteries.

A Low Temperature Soldered All Ceramic Lithium Battery.

The oxide-based all ceramic lithium battery (ACLB) is regarded as one of the safest secondary batteries because it is incombustible and free of toxic gas release. However, high temperature sintering is a necessary step to fabricate the solid-state electrolytes (SSEs) membranes and improve the cathode/SSEs interfacial contact, which bring in high energy consumption as well as the formation of Li-ion resistive interdiffusion phases. Here, we report an in situ coating of lithium-rich antiperovskites (LiRAPs) as sintering aids to solder LiCoO2 (LCO) active material and Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid electrolyte. Due to the low melting point of LiRAPs (273.2 °C), all particles were compactly soldered to simultaneously densify the electrolyte membrane and reinforce the cathode/electrolyte contact, thus lowing the sintering temperature of ACLB from over 600 °C to only 290 °C. The interfacial resistance of cathode/electrolyte was reduced from 15 288 to 817 Ω/cm2 due to the high ionic conductivity of LiRAPs and the interdiffusion phases prohibition. Moreover, the outstanding ductility of LiRAPs also mitigated the strain/stress of the LCO/LATP interface, which lead to improved cycling stability. These results not only provide a rational design to the cathode/SSEs interface but also deliver a practical stacking process to speeding up the industrialization of ACLB.