Surface Of Solid Electrolyte Research Articles

A New General Paradigm for Understanding and Preventing Li Metal Penetration through Solid Electrolytes

Summary The use of lithium (Li) or sodium (Na) metal anodes together with highly ion-conductive solid electrolytes (SEs) could provide batteries with a step improvement in volumetric and gravimetric energy densities. Unfortunately, these SEs face significant technical challenges, in large part because Li and Na dendrites can penetrate through SEs, leading to short circuits. The ability of such a soft material (Li or Na metal) to penetrate through ceramic is surprising from the point of view of models widely used in the Li-battery field. We introduce a concept, new to the battery field, for preventing penetration of lithium dendrites through SEs by putting the SE surfaces into a state of residual compressive stress. For a sufficiently high compressive stress, cracks have difficulty forming, and cracks that do form are forced to close, inhibiting dendrite penetration. This approach is widely used to solve commercially important stress corrosion cracking problems in metals and static fatigue problems in ceramics and glasses (e.g., Gorilla Glass). However, the technique will not be useful for SEs if the Li-ion transport rate through a SE is substantially reduced when the SE is under compression. Our molecular dynamics calculations for Li-ion transport through a common SE demonstrate that the introduction of even very high residual compressive stresses (∼10 GPa) has only a modest effect on Li-ion transport kinetics, suggesting that this approach is viable and capable of providing a new paradigm for developing high-performance and mechanically stable SEs.

A review of gas evolution in lithium ion batteries

This is a review on recent studies into the gas evolution occurring within lithium ion batteries and the mechanisms through which the processes proceed. New cathode materials such as lithium nickel manganese cobalt oxides are being heavily researched for the development of higher specific capacity electrodes. These materials often suffer from rapid degradation which coincides with gas evolution. Further sources of gas evolution include electrolyte reduction at the anode during the initial cycles culminating in formation of a solid electrolyte interphase and surface layer compounds formed on the cathode during production and storage. There have been several techniques established for detection and quantification of gas evolution in ex situ and in situ studies, primarily gas chromatography mass spectrometry and differential/on-line electrochemical mass spectrometry.

Sandwich structured NASICON-type electrolyte matched with sulfurized polyacrylonitrile cathode for high performance solid-state lithium-sulfur batteries

• High performance sandwich structured SPE-LATP-SPE electrolyte was prepared. • SPAN anode was successfully applied to all-solid-state lithium-sulfur batteries. • The SPAN|SPE-LATP-SPE|Li batteries exhibited excellent electrochemical performance. • Interface reaction between LATP and lithium anode was suppressed. All-solid-state lithium-sulfur batteries show increasing potential for practical applications in portable electronic devices and electric vehicles due to their high energy density, low cost, and environmental friendliness. However, the large interface impedance of solid-state lithium-sulfur batteries leads to low capacity and short cycle life. In this study, a hierarchical design of sandwiched NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) solid-state electrolyte with surface modification by a solid polymer electrolyte (SPE) is proposed for high-performance lithium-sulfur batteries. Due to the unique hierarchical structure of the solid electrolyte in which SPE (PEO: LiTFSI = 8:1) layer is coated on NASICON solid electrolyte surface, the direct contact between lithium metal anode and LATP solid electrolyte can be avoided, and the improved interfacial property between the electrolyte and electrodes can be achieved. As a result, the as-prepared solid-state Li|SPE-LATP-SPE|Li symmetrical cell exhibits a stable cycling performance. Moreover, solid-state lithium-sulfurized polyacrylonitrile (SPAN) battery based on such electrolyte delivers an ultrahigh initial discharge capacity of 1793 mAh g −1 at 75 °C with high coulombic efficiencies and stable cycling performance. The present work provides a creative design of battery configuration for manufacturing high-performance and safe solid-state lithium-sulfur batteries.

Перспективные осмотическая и гибридная электрохимическая электростанции

A range of energy technologies ultimately aimed at obtaining electric energy is considered. Proceeding from the list of considered sources, it is possible to analyze their different combinations for achieving better energy efficiency of new complexes. A systematic list of 21 currently known traditional, non-traditional, and renewable energy sources is compiled. Each of them taken individually has an efficiency not exceeding 50%, except for some types of fuel cell based power facilities. Block diagrams of energy flow conversion stages are proposed for the considered kinds of sources. Obviously, if some or other chain does not contain certain blocks in comparison with the first classical chain of thermal engine thermodynamic cycles, this means that the missing energy conversion stages of are either implemented covertly, or proceed in the environment. As an example, two promising sources are considered: an osmotic hydroelectric power plant and a hybrid power plant (HybPP) based on high-temperature fuel cells with solid oxide electrolyte and a gas turbine unit. In fact, an osmotic hydroelectric power plant takes the solar energy spent for evaporation from sea surfaces in the form of the osmotic pressure phenomenon energy under the conditions of one-way diffusion of fresh river water (a solvent) molecules through a semi-permeable membrane towards salt sea water (a solution). An osmotic HPP is a combination of a reservoir with semi-permeable membranes and an HPP. The former is characterized by the expected high specific power up to 12 kW per square meter of semi-permeable membrane area, and the latter is characterized by the highest efficiency among all types of electric power sources and by the high achieved specific power up to 2-3 kW per square meter of solid oxide electrolyte surface area.

The Active Interface of Ta-Doped Li7La3Zr2O12 for Li Plating/Stripping Revealed by Acid Aqueous Etching

All-solid-state lithium batteries incorporating oxide-based solid electrolytes have attracted much attention as a promising battery system for enabling highly reversible Li metal anodes. However, the cycling stability of Li plating/stripping reactions at higher charging/discharging rates on garnet-type solid-state electrolytes must be improved to realize a practical Li metal anode for solid-state batteries. Here, we report that a short acid etching procedure performed in ambient air significantly activates the Ta-doped Li7La3Zr2O12 (LLZT) surface compared to polishing under inert gas atmosphere such as dry Ar. It has been believed that Li7La3Zr2O12 (LLZ) and related doped LLZ solid electrolyte surfaces need to be mechanically polished in dry Ar before the cell fabrication to remove Li2CO3 and LiOH that are present on the surface. However, a commonly used mechanical polishing procedure is found to form a thin electrochemically inactive layer on the LLZT surface, whereas a short acid etching procedure (e.g., HCl) removes the inactive layer, and the acid-etched LLZT exhibits excellent cycling stability.

Stability of composite electrolytes based on Li7La3Zr2O12 to metallic lithium

The stability of the composite electrolytes based on tetragonal and cubic modification of Li7La3Zr2O12 with 65Li2O·27B2O3·8SiO2 or 40.2Li2O·5.7Y2O3·54.1SiO2 glass addition versus metallic lithium in stationary conditions and under constant current applied is studied in the paper. A complex of electrochemical techniques established the growth of symmetric cell resistance and overvoltage in measuring cell for composites based on tetragonal Li7La3Zr2O12, which denotes the degradation of the solid electrolyte surface for tetragonal Li7La3Zr2O12–x wt% glass electrolytes due to the formation of the impurities confirmed by XRD. The resistance of the symmetric cells with composite electrolytes based on cubic modification of Li7La3Zr2O12 does not change in the course of the experiment and the voltage reaches the plateau at constant current applied. Thus, composites based on the cubic Li7La3Zr2O12 with a small addition of lithium boron-silicate and yttrium-silicate glasses are stable versus lithium. Moreover, the cross section of the samples remains white colored after electrical testing and no dendrite formation is observed.

Rate-Limiting Factors in Oxygen Transfer through Electrochemical Oxygen Pump in Liquid LBE

This paper presents the polarization characteristics of electrochemical oxygen pumps (EOPs) during transfer oxygen from/to liquid lead-bismuth eutectic (LBE). A thick-walled (1.5 mm) one-end closed tube of yttria partially stabilized zirconia was used as a solid electrolyte. Three different electrode of air/LSM (lanthanum strontium manganite), air/LSCF (lanthanum strontium cobalt ferrite) and LBE/PbO were compared. The polarization characteristics were obtained by linear sweep voltammetry in LBE at 450°C at various dissolved oxygen concentrations in LBE. The EOP with LBE/PbO electrode showed negligible activation polarization compared to EOPs with other electrodes. However, with the LBE/PbO electrode a significant concentration polarization occurred at low current density, limiting its capacity for oxygen transfer from EOP to LBE. The oxygen transfer from LBE to EOP is limited by oxygen mass transfer from the LBE bulk to the solid electrolyte surface of EOPs, especially under low dissolved oxygen condition.

Nano-scale oxide formation inside electrochemically-formed Pt blisters at a solid electrolyte interface

We report on platinum oxide formation during electrochemical anodic polarization of a platinum film on yttria-stabilized zirconia (YSZ) under electrochemical oxygen potential control. The electrochemical potential drives oxygen through the YSZ electrolyte towards a nominally 175 nm thin Pt film, which we found to locally delaminate from the substrate by forming nano-scale blisters. High resolution scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDX) mapping of focused-ion beam (FIB)-prepared cross-sections of single bubbles of a few micrometers in diameter reveal them to be hollow and enclosed by a Pt outer and a few tens of nanometers thick PtOx inner shell. The oxide shell presumably formed due to the increase of local oxygen chemical activity under the applied process conditions (723 K, 500 mbar O2, bias voltage +100 mV). Interface X-ray diffraction indicates that the solid electrolyte surface morphology is largely unaffected by the process suggesting that the YSZ surface is stable on the atomic scale under application relevant oxygen transport conditions. Platinum is known to be rather stable towards oxidation, even at elevated oxygen pressure, leading to oxide-scale thicknesses of the order of 1 nm. Our results however indicate that many of the kinetic barriers for oxidation during the nano-confined blistering process are lowered. This may have implications in general for the mechanism how oxygen is stored in an electrode at such an internal metal - oxide/metal - gas interface, which is important for the functionality of many solid-state electrochemical and memresistive devices.

Peering through the Stability Window

In the December issue of Chem, Feng Pan and colleagues perform a detailed study of a super-concentrated aqueous lithium-ion battery electrolyte that more than doubles the intrinsic electrochemical window of water (2.55 V compared to 1.23 V). From molecular dynamics simulations, combined with a suite of extensive characterization methods and electrochemical measurements, the authors correlate the local atomic structure of aqueous LiNO3 electrolyte to its observed enhanced electrochemical stability. They ultimately determine that the increased energy barrier for bulk water desolvation due to super-concentration is primarily responsible.

Safety First

Safety First

Thin Film Surface Coatings for Improved Lithium Metal Cycling Efficiency: A Combinatorial Approach

There is a continual push to improve the energy density of lithium-ion batteries, but this is becoming increasingly difficult as it is believed that many of the best electrode materials have been found and optimized. In order to achieve higher energy densities to meet future storage demands it may be necessary to move “beyond lithium-ion”. Recent research efforts have focused on reviving the lithium metal negative electrode as a potential path to higher energy density.[1] With its high theoretical capacity and lowest reduction potential among metals, using lithium as a negative electrode can certainly increase the energy density of a cell provided the large volume changes of the lithium electrode between the charged and discharged states can be handled. In addition, lithium metal anodes often demonstrate dendrite formation during electrodeposition instead of plating as a smooth film. Since conventional organic electrolytes are thermodynamically unstable to reduction by lithium, dendrite growth leads to continual loss of active lithium, resulting in poor cycling efficiencies (< 90%) and short cell lifetime.[2] These problems are exaggerated as the thickness of the plated lithium increases, making cells with industrially relevant material loadings a significant challenge. Recent studies have shown that the morphology and plating efficiency of lithium can be greatly improved with nanostructured surface coatings. [3],[4] Herein we report on the use of combinatorial materials analysis to investigate the effect of different nanostructured surface coatings on the electrochemical deposition of lithium metal. Custom 64-channel electrochemical cell plates were used along with a combinatorial electrochemical cell to provide an efficient means of screening different electrode coatings. Figure 1 shows a schematic of the 64-channel cell plate as well as the output cyclic voltammograms (CVs) from potentiodynamic lithium plating and stripping on 64 unmodified copper electrodes. All 64 channels show consistent output which was validated against conventional coin type lithium half cells. High throughput sputtering was used to make libraries of thin films with different composition, structure, and thickness. These sputtered libraries were deposited directly on the 64-channel cell plates and used to analyze the morphology and coulombic efficiency of lithium plating as a function of the 64 individual surface coatings. The influence of different electrolyte compositions with these surface coatings was also investigated. These results provide perspective regarding the value of different thin film anode surface coatings as part of a broad strategy for achieving high (>98 %) lithium metal cycling efficiencies. [1] X. Cheng et al., Toward safe lithium metal anode in rechargeable batteries: a review, Chemical reviews, 117 (2015), 10403-10473. [2] Q. Pang, et al. "An In Vivo Formed Solid Electrolyte Surface Layer Enables Stable Plating of Li Metal." Joule 1, (2017): 871-886. [3] Adam P. Cohn et al., Anode-Free Sodium Battery through in Situ plating of Sodium Metal, Nano Letters, 17, (2017) 1296-1301. [4] G. Zheng et al., Interconnected hollow carbon nanospheres for stable lithium metal anodes, Nature Nanotechnology 9, (2014), 618-623. Figure 1

Electrochemical Properties of Composite Cathode Materials Pr1.95La0.05CuO4–Ce0.9Gd0.1O1.95 for Intermediate Temperature Solid Oxide Fuel Cells

The electrochemical properties are studied for composite electrodes Pr1.95La0.05CuO4(PLCO)–xCe0.9Gd0.1O1.95(GDC), where x = 20, 30, 40, and 50 wt % GDC with the aim of finding the composition with the best electrochemical efficiency in the oxygen reduction reaction. Varying the temperature of sintering of the PLCO–xGDC electrode layer to the surface of GDC solid electrolyte shows that the minimum polarization resistance (Rη) is reached at the temperature of 850°C. For the PLCO–xGDC composition containing 40 wt % GDC, in the temperature range of 600–750°C, the maximum electrochemical activity in oxygen reduction reaction is observed as indicated by 10-fold decrease in Rη as compared with single-phase PLCO (from 0.87 (x = 0) to 0.08 Ω cm2 (x = 40) at 700°C in air). According to the data obtained, the PLCO–40GDC composite can be considered as a promising cathode material for intermediate temperature solid oxide fuel cells.

(Invited) Reactions or No Reaction: Lithium Deposition on the Surface of Solid State Electrolyte

Li metal anode has regained intensive interest in recent years in order to develop high energy next-generation battery technologies. Unfortunately, Li metal suffers from poor cycling stability and low efficiency as well as the formation of dangerous Li dendrites raising safety concerns. The employment of solid state electrolyte (SSE) to prevent Li dendrite growth provides a promising approach to address the dendrite issue. However, recent studies indicate that Li dendrites easily form at elevated current densities, while the fundamental mechanisms of forming Li dendrites within SSE is still unknown. This calls for further investigation to understand, and control the detrimental observation. The origin and evolution of Li dendrite growth through SSE will be discussed in this talk by using two different SSE membranes, garnet and phosphate-type, as the separators. During cycling, Li is repeatedly deposited on SSE. Although a good SSE should not react with the deposited Li, the reactions between Li deposits and SSE generate a self-terminating interface, which stops the fast propagation of dendritic Li through the SSE membrane. New insights are provided on the further modification and/or incorporation of interfacial layers between SSE and Li metal to enable future solid state batteries.

Development of lanthanum-doped praseodymium cuprates as cathode materials for intermediate-temperature solid oxide fuel cells

Electrochemical properties of the Pr2-xLaxCuO4 (x = 0.05; 0.1; 0.3) (PLCO) oxides in oxygen reduction reaction (ORR) were examined towards their applicability as cathode materials for intermediate-temperature solid oxide fuel cells (IT-SOFCs). Pr1.95La0.05CuO4 (PLCO0.05) was defined as a favorable basis for the composite cathode material due to its conducting, thermomechanical and electrocatalytic properties. The optimization of the annealing temperature of the PLCO0.05-xGDC composite electrode deposited on GDC solid electrolyte surface had shown that the lowest area specific resistance (ASR) was achieved at 850 °C. The highest electrochemical activity in ORR was achieved for the composition containing 40 wt% GDC in the temperature range of 600–750 °C. The application of PLCO0.05-40GDC composite cathode instead of pure PLCO0.05 made it possible to reduce ASR up to 10 times at 700 °C in air (from 0.87 Ω·cm2 (x = 0 wt%) to 0.08 Ω·cm2 (x = 40 wt%)). According to the data obtained, PLCO0.05-40GDC can be considered as a promising cathode material for IT-SOFCs.

Lithium Metal Anodes: A Recipe for Protection

Effective stabilization of lithium metal anode is the key to the development of next-generation high-energy rechargeable batteries. In this issue of Joule, Linda Nazar and colleagues demonstrated a rationally designed electrolyte additive that can form a robust, single-ion-conducting protective layer on lithium metal surface while the battery operates, promoting uniform lithium deposition with high cycling efficiency.

Transient Behavior of the Metal Interface in Lithium Metal-Garnet Batteries.

The interface between solid electrolytes and Li metal is a primary issue for solid-state batteries. Introducing a metal interlayer to conformally coat solid electrolytes can improve the interface wettability of Li metal and reduce the interfacial resistance, but the mechanism of the metal interlayer is unknown. In this work, we used magnesium (Mg) as a model to investigate the effect of a metal coating on the interfacial resistance of a solid electrolyte and Li metal anode. The Li-Mg alloy has low overpotential, leading to a lower interfacial resistance. Our motivation is to understand how the metal interlayer behaves at the interface to promote increased Li-metal wettability of the solid electrolyte surface and reduce interfacial resistance. Surprisingly, we found that the metal coating dissolved in the molten piece of Li and diffused into the bulk Li metal, leading to a small and stable interfacial resistance between the garnet solid electrolyte and the Li metal. We also found that the interfacial resistance did not change with increase in the thickness of the metal coating (5, 10, and 100 nm), due to the transient behavior of the metal interface layer.

Transient Behavior of the Metal Interface in Lithium Metal–Garnet Batteries

AbstractThe interface between solid electrolytes and Li metal is a primary issue for solid‐state batteries. Introducing a metal interlayer to conformally coat solid electrolytes can improve the interface wettability of Li metal and reduce the interfacial resistance, but the mechanism of the metal interlayer is unknown. In this work, we used magnesium (Mg) as a model to investigate the effect of a metal coating on the interfacial resistance of a solid electrolyte and Li metal anode. The Li–Mg alloy has low overpotential, leading to a lower interfacial resistance. Our motivation is to understand how the metal interlayer behaves at the interface to promote increased Li‐metal wettability of the solid electrolyte surface and reduce interfacial resistance. Surprisingly, we found that the metal coating dissolved in the molten piece of Li and diffused into the bulk Li metal, leading to a small and stable interfacial resistance between the garnet solid electrolyte and the Li metal. We also found that the interfacial resistance did not change with increase in the thickness of the metal coating (5, 10, and 100 nm), due to the transient behavior of the metal interface layer.

Effect of samaria-doped ceria (SDC) interlayer on the performance of La0.6Sr0.4Co0.2Fe0.8O3-δ/SDC composite oxygen electrode for reversible solid oxide fuel cells

In order to establish clear criteria for designing highly active and highly durable oxygen electrode for reversible solid oxide fuel cells, we have focused on the effect of samaria-doped ceria (SDC) interlayers prepared on YSZ solid electrolyte surface on the performances of La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF)-SDC composite oxygen electrode. Symmetrical cells with the configuration, LSCF-SDC|SDC interlayer|YSZ|SDC interlayer|LSCF-SDC, were constructed. We prepared two kinds of SDC interlayers, one from a mixed solution of cerium 2-ethylhexanoate (denoted as octoate) and samarium octoates (o-interlayer) and another from a mixed solution of cerium and samarium nitrates (n-interlayer). The LSCF-SDC electrodes with o-interlayer and n-interlayer exhibited very similar performances in both the anodic and cathodic reactions at 900°C. When temperature was decreased to 800°C, an increase in overpotentials was observed. However, the LSCF-SDC electrode with o-interlayer exhibited superior performance to that with n-interlayer. It was found that the entire surface of the YSZ electrolyte disk was well covered with a dense o-interlayer of uniform thickness. Such an interlayer enables uniform transport of oxide ions to and from the LSCF-SDC electrode, resulting in an enlarged effective reaction zone (ERZ). The I-E performance of the LSCF-SDC|o-interlayer|YSZ cell was found to be comparable to that of the identical electrode prepared on a dense SDC sintered electrolyte disk (as a reference). This observation supports our views regarding the essential role of a dense interlayer with uniform thickness in enhancing the performance of reversible solid oxide cells.

Local Structure and Composition Variation at Surface of Lithium-Ion Conducting Solid Electrolyte

Recently, lithium ion conducting solid electrolytes attract many interests because of their potential application to all-solid-state batteries (ASSBs), which are supposed to be one of candidates of next-generation energy storage devices with high safety and reliability [1-3]. With great efforts of development of solid electrolytes, several materials with high lithium ionic conductivity have been reported, which facilitated hope of realization of ASSBs [2,4-8]. Now, researchers face several problems on application of solid electrolytes to ASSBs. Most of those problems are related to interfaces of between solid electrolytes and active materials, for example, contact areas, interdiffusion of elements on assembly and/or electrochemical processes of ASSBs. To solve these issues, much attention has been paid to design and fabrication techniques. In addition to the problems on the fabrication, several reports point out intrinsic phenomena related change in ion concentration at interfaces of solid electrolytes [1, 9, 10]. We have so far studied the local structure at the interfacial region by fabricating nano-composites of active materials and solid electrolytes, and confirmed that the interfacial region with distorted lattice ranges for at least 20-50 nm in thickness [9, 10]. Although more researches with variety of experimental analysis are required for further comprehension of the interfacial phenomena, difficulty in the analysis of solid/solid interface limits experimental tools. It is known that surface of solid electrolytes is also related to interfacial resistance. Kliewer proposed cation depletion at surface of ionic crystals when free energy of defect formation is lower for cation than for anion [11]. In addition, we observed that ball-milling of a poor ionic conductor (Li2SiO3, LSO) resulted in increase in ionic conductivity without change in activation energy [9, 12]. In this study, three different surface-sensitive techniques, grazing incidence X-ray diffraction (GIXD), attenuated total reflectance Fourier transform infrared (ATR-FTIR), and X-ray photoelectron spectroscopy (XPS), were employed to analyze the local structure and composition around the surface region of a lithium ion conducting solid electrolyte sheet (NASICON-type in the system of Li-Al-Ti-Ge-Si-P-O, Ohara Inc. abbreviated as LICGC). It was revealed that the local structure and composition changed depending on depth from the top surface of the sheet. At the very surface, there was a layer with expanded lattice (Figure 1) and high Li composition (Figure 2). And with increasing the depth from the surface, lattice shrank sharply, and then expanded again gradually. The change in the lattice seemed to be accompanied by Li and Al composition. It was supposed that the change in the Li composition and structure is induced by combination of chemical reaction, segregation, and defects distribution [13].

3D Printing Microstructured Li-Garnet Electrolytes for Solid-State Lithium Batteries

Recent advancements in solid electrolytes have brought all solid-state lithium batteries much closer to a commercial reality. Lithium garnet materials such as Li7La3Zr2O12, or LLZ, are ceramic lithium conductors that have several uniquely advantageous properties: they are completely non-flammable, low cost to produce, and stable to lithium metal, which has an energy density more than 10x higher than standard graphite electrodes (3860 mAh/g). The main areas challenging the development of all-solid-state Li-ion batteries, however, have been relatively low ionic conductivity compared organic liquid electrolytes (~1 mS/cm compared to 10 mS/cm) and high interfacial impedance due, in part, to poor solid-solid contact at the electrolyte/electrode interface. However, by controlling the thickness of the electrolyte separating the two electrodes down to the order of tens of microns, the contribution of the conductivity to the overall resistance of the bulk electrolyte can become negligible. To address the interfacial impedance requires tailoring the architecture of the electrolyte surface to maximize accessible interfacial area and reduce the resistance for Li+ cation transfer at that interface. Using an advanced 3D printer, different approaches were taken to optimize fabrication of both thin, low resistance solid electrolyte films and films with sophisticated surface microstructures. The creation of various geometries (e.g., grid patterns, multilayer structures, etc.) and their impact on pore structure and interfacial area was investigated in depth and will be discussed. Furthermore, electrodes were infiltrated into each of the pore structures and analyzed using SEM to determine which geometry facilitated the most extensive and intimate electrode-electrolyte contact. As a demonstration of the potential impact of microstructured solid electrolytes, electrochemical testing results of the 3D printed ordered structures was compared with the random-porosity structures of the same material created by tapecasting. The ordered microstructures consistently delivered better performance due to improved electrode-electrolyte contact. This work sheds light on the importance of the solid electrolyte surface, and how tuning its structure can help to overcome the challenges of solid-state batteries.