The commercialization of rechargeable lithium-ion batteries (LIBs) has revolutionized the modern lifestyle, [1] leading society into an electrified, wireless, and sustainable future. With the continuous upsurge in demand for energy-dense devices, future advancement of batteries will require higher energy density, longer cycle life, and better safety. [2,3] Lithium metal anodes have a high specific capacity of ≈3800 mAh g −1 , [4,5] enabling the possibility of higher energy density batteries. However, commonly used liquid electrolytes in Li metal batteries (LMBs) often result in uncontrollable lithium dendrite growth, inadequate electrochemical and thermal stability, and high flammability. [2,4] As a result, limited performance and safety issues restrict the application and development of LMBs based on conventional liquid electrolytes.Compared to liquid electrolytes, solidstate electrolytes (SSEs) can potentially provide better safety, higher mechanical strength, and excellent chemical and electrochemical stability. [4,[6][7][8][9][10] SSEs can be grouped into three categories: inorganic solid electrolytes, [11][12][13][14] solid polymer electrolytes (SPEs), [15][16][17] and their hybrids. [18][19][20][21] Among them, inorganic solid electrolytes have the highest ionic conductivity [11] and excellent thermal stability, [2] but their interfacial compatibility, brittleness, and rigidity [22,23] are the challenges to be addressed towards their practical application. [9] In contrast, SPEs have good interfacial compatibility, [24] and excellent chemical and electrochemical stability, [18,24,25] but are lacking in thermal stability and mechanical strength, which generally makes them insufficient for meeting the requirements of high-safety and high-performance LMBs, [6,26,27] especially at high temperatures (>100 °C). [28] A hybrid of ceramic and polymer SSEs may offer good mechanical strength and safety, but it is still challenging to achieve ultrathin composite SSEs. Therefore, the design of a robust, ultrathin SSE that fulfills the above requirements is urgently needed.To achieve an energy density comparable to or larger than liquid electrolyte-based cells, ultrathin and lightweight solid electrolytes are necessary. [29,30] Compared to typical, thick ceramic electrolytes with thicknesses in the range of a few hundred microns, [14,[31][32][33] SPEs and their composites are easily engineered and manufacturable for tunable smaller All-solid-state batteries (ASSBs) demonstrate great promise, offering high energy density, good thermal stability, and safe operation compared with traditional Li-ion batteries. Among various solid-state electrolytes (SSEs), solid polymer electrolytes (SPEs) offer an attractive choice due to their thinness, low density, and good manufacturability. However, ultrathin SPEs that work with practical current densities or at high temperatures remain challenging, limiting applicable conditions of SPE-based batteries. Here, the authors report a novel scalable, ultrathin, and high-temperature-resistant ...

batteries (ASSBs) using the inorganic SSE and Li-metal anode still experience issues with dendrite penetration and associated early short-circuit during battery operation. [11][12][13][14] So far, considerable efforts have been devoted to elucidating the underlying mechanisms of this early failure of ASSBs. [15][16][17][18] It is generally acknowledged that the dynamic morphological evolution at the Li/SSE interface can remarkably influence the electrochemical performance of ASSBs. [17,[19][20][21][22][23] In specific, during striping, Li atoms at the Li/SSE interface dissolve into SSE, and meanwhile, the diffusion of Li atoms in Li metal replenishes the Li loss from the interface. Since the rate of Li striping usually exceeds the diffusion limit of Li atoms, the Kirkendall voids will initiate and grow at the interface, leading to the loss of interfacial contact and increased cell impedance. [20,24,25] The morphological degradation becomes even worse during the subsequent plating. Li prefers to deposit at the regions still contacted with SSE instead of the detached areas, which develops a nonuniform deposition at the interface that further promotes the nucleation and growth of Li dendrites as well as the short-circuit of ASSBs. [22,26] An effective strategy to inhibit morphological degradation at the Li/SSE interface is applying an external stack pressure on ASSBs. [20][21][22] With the pressure, Li metal near the interface can mechanically deform through creep, offering another route to replenish the Li loss and thus prevent the void formation. [21,27] Nevertheless, the practical adoption of this strategy is limited by a strict constraint from the "critical stack pressure." [20] In specific, the applied pressure has to be higher than the "critical stack pressure" to effectively suppress the morphological degradation at the interface. Otherwise, the mechanical deformation will be slower than the electrochemical deformation caused by Li stripping, leading to an insufficient Li replenishment to the interface. In this case, the voids will still form at the interface, followed by the nucleation and growth of Li dendrites (Figure 1a). It should be noticed that the "critical stack pressure" can reach several MPa for the ASSBs cycled under relatively low current density (e.g., 7.5 MPa for the Li/garnet/ Li cell cycled under 0.2 mA cm -2 ). [20,21,28] This high stack pressure is out of range of the current LIB operation platform (0.1-1.0 MPa) [29] and also sets constraints on the robustness of SSE and thus the broad adoption of viable SSE. [29] Moreover, it is possible that the pressure of this magnitude acts as one Morphological degradation at the Li/solid-state electrolyte (SSE) interface is a prevalent issue causing performance fading of all-solid-state batteries (ASSBs). To maintain the interfacial integrity, most ASSBs are operated under low current density with considerable stack pressure, which significantly limits their widespread usage. Herein, a novel 3D-micropatterned SSE (3D-SSE) that can stabilize the morpho...

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A new mixed solvent enables rapid fabrication of high-quality perovskite films directly by one-step spin-coating or blade-coating.

Oriented graphene foam performs well in inhibition of Li dendrite formation at 1, 2 and 5 mA cm−2 as a current collector.

High-performance, practical all-solid-state batteries (ASSBs) require solid-state electrolytes (SSEs) with fast Li-ion conduction, wide electrochemical stability window, low cost, and low mass density. Recent density functional theory (DFT) simulations have suggested that lithium thioborates are a particularly promising class of materials for high-performance SSEs in Li batteries, but these materials have not been studied extensively experimentally due to synthesis difficulty. Particularly, their electrochemical properties remain largely underexplored, limiting their further development and application as SSEs. In this work, we report the successful synthesis and a comprehensive electrochemical performance study of single-phase, crystalline Li6+2x [B10S18]­S x (x ≈ 1). We find cold-pressed samples of Li6+2x [B10S18]­S x (x ≈ 1) to exhibit a high ionic conductivity of 1.3 × 10–4 S cm–1 at room temperature. Furthermore, Li6+2x [B10S18]­S x (x ≈ 1) shows an electrochemical stability window of 1.3–2.5 V, much wider than most sulfide SSEs. Symmetrical Li–Li cells fabricated with a Li6+2x [B10S18]­S x (x ≈ 1) pellet were cycled up to a current density of 1 mA cm–2 and exhibited good long-term cycling stability for more than 140 h at 0.3 mA cm–2. These results suggest Li6+2x [B10S18]­S x (x ≈ 1) as a promising choice of SSE for high-performance ASSBs for energy storage.

All‐solid‐state lithium metal batteries are prominent candidates for next‐generation batteries with high energy density and low safety risks. However, the traditional planar contact between Li metal and solid‐state electrolytes (SSEs) exhibits substantive void formation and large interfacial morphological fluctuation, causing poor interfacial stability. Here, an interdigitated Li‐solid polymer electrolyte framework (I‐Li@SPE), a pioneering demonstration of 3D interface in polymer‐based all‐solid‐state batteries, is designed, transferring the Li‐SSE interfacial contact from planar to 3D for enhanced interfacial integrity. A smooth and intact 3D Li‐SSE interfacial contact after repeated cycling that precedes planar Li‐SSE contact, is shown. COMSOL simulation indicates I‐Li@SPE reduces local current densities by more than 40% and moderates interfacial variation by more than 50%. As a result, I‐Li@SPE achieves high critical current density of 1 mA cm−2, as well as promising high areal capacity cycling of 4 mAh cm−2 at 0.4 mA cm−2. This work provides a new structure for Li‐SSE composite fabrication and high‐capacity solid‐state Li batteries.

Load bearing/energy storage integrated devices (LEIDs) allow using structural parts to store energy, and thus become a promising solution to boost the overall energy density of mobile energy storage systems, such as electric cars and drones. Herein, with a new high-strength solid electrolyte, we prepare a practical high-performance load-bearing/energy storage integrated electrochemical capacitors with excellent mechanical strength (flexural modulus: 18.1 GPa, flexural strength: 160.0 MPa) and high energy storage ability (specific capacitance: 32.4 mF cm−2, energy density: 0.13 Wh m−2, maximum power density: 1.3 W m−2). We design and compare two basic types of multilayered structures for LEID, which significantly enhance the practical bearing ability and working flexibility of the device. Besides, we also demonstrate the excellent processability of the LEID, by forming them into curved shapes, and secondarily machining and assembling them into complex structures without affecting their energy storage ability.