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The garnet electrolyte presents poor wettability with Li metal, resulting in an extremely large interfacial impedance and drastic growth of Li dendrites. Herein, a novel ultra‐stable conductive composite interface (CCI) consisting of LiySn alloy and Li3N is constructed in situ between Li6.4La3Zr1.4Ta0.6O12 (LLZTO) pellet and Li metal by a conversion reaction of SnNx with Li metal at 300 °C. The LiySn alloy as a continuous and robust bridge between LLZTO and Li metal can effectively reduce the LLZTO/Li interfacial resistance from 4468.0 Ω to 164.8 Ω. Meanwhile, the Li3N as a fast Li‐ion channel can efficiently transfer Li ions and give their uniform distribution at the LLZTO/Li interface. Therefore, the Li/LLZTO@CCI/Li symmetric battery stably cycles for 1200 h without short circuit, and the all‐solid‐state high‐voltage Li/LLZTO@CCI/LiNi0.5Co0.2Mn0.3O2 battery achieves a specific capacity of 161.4 mAh g−1 at 0.25 C with a capacity retention rate of 92.6 % and coulombic efficiency of 100.0 % after 200 cycles at 25 °C. [ABSTRACT FROM AUTHOR]

The garnet electrolyte presents poor wettability with Li metal, resulting in an extremely large interfacial impedance and drastic growth of Li dendrites. Herein, a novel ultra‐stable conductive composite interface (CCI) consisting of LiySn alloy and Li3N is constructed in situ between Li6.4La3Zr1.4Ta0.6O12 (LLZTO) pellet and Li metal by a conversion reaction of SnNx with Li metal at 300 °C. The LiySn alloy as a continuous and robust bridge between LLZTO and Li metal can effectively reduce the LLZTO/Li interfacial resistance from 4468.0 Ω to 164.8 Ω. Meanwhile, the Li3N as a fast Li‐ion channel can efficiently transfer Li ions and give their uniform distribution at the LLZTO/Li interface. Therefore, the Li/LLZTO@CCI/Li symmetric battery stably cycles for 1200 h without short circuit, and the all‐solid‐state high‐voltage Li/LLZTO@CCI/LiNi0.5Co0.2Mn0.3O2 battery achieves a specific capacity of 161.4 mAh g−1 at 0.25 C with a capacity retention rate of 92.6 % and coulombic efficiency of 100.0 % after 200 cycles at 25 °C. [ABSTRACT FROM AUTHOR]

The interfacial issues between garnet electrolyte and Li metal hinder the application of garnet electrolyte in solid-state Li metal batteries. Herein, a three-dimensional (3D) porous Zn layer (PZL) is magnetron sputtered on the surface of Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) to construct a 3D Li–Zn alloy layer at the LLZTO/Li interface by melting Li metal into PZL. The 3D Li–Zn alloy effectively reduces the LLZTO/Li interfacial impedance from 319.8 Ω cm2 to an extremely low value of 1.9 Ω cm2. Meanwhile, the 3D alloy skeleton can enhance the transport kinetics and promote uniform distribution of Li ion at interface to inhibit the growth of Li dendrites. More importantly, the volume expansion of interface between LLZO and Li metal anode is effectively suppressed due to the host role of 3D Li–Zn alloy interface. The Li/LLZTO@PZL/Li symmetrical battery achieves a high critical current density of 2 mA cm−2 for one cycle. The all-solid-state LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523)/LLZTO@PZL/Li battery with a high cathode loading of 4.9 mg cm−2 delivers a high specific capacity of 143.8 mAh g−1 after 170 cycles. The 3D alloy interface is significant for enhancing the interfacial stability of high capacity all-solid-state lithium metal batteries. • A 3D Li–Zn alloy layer is constructed at Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 /Li interface. • The 3D interface can reduce interfacial impedance from 319.8 to 1.9 Ω cm2. • The 3D interface achieves a critical current density of 2 mA cm−2. • The 3D interface enables high-loading solid LiNi 0.5 Co 0.2 Mn 0.3 O 2 /Li battery. [ABSTRACT FROM AUTHOR]

This work verifies the Li-ion transfer of ceramic electrolytes in ceramic-liquid hybrid electrolytes during battery cycling and also finds spontaneous Li-ion exchange between ceramic and liquid electrolytes through tracking the 6Li and 7Li substitution behavior using solid-state nuclear magnetic resonance (NMR) spectroscopy. [Display omitted] Ceramic electrolytes are important in ceramic-liquid hybrid electrolytes (CLHEs), which can effectively solve the interfacial issues between the electrolyte and electrodes in solid-state batteries and provide a highly efficient Li-ion transfer for solid–liquid Li metal batteries. Understanding the ionic transport mechanisms in CLHEs and the corresponding role of ceramic electrolytes is crucial for a rational design strategy. Herein, the Li-ion transfer in the ceramic electrolytes of CLHEs was confirmed by tracking the 6Li and 7Li substitution behavior through solid-state nuclear magnetic resonance spectroscopy. The ceramic and liquid electrolytes simultaneously participate in Li-ion transport to achieve highly efficient Li-ion transfer in CLHEs. A spontaneous Li-ion exchange was also observed between ceramic and liquid electrolytes, which serves as a bridge that connects the ceramic and liquid electrolytes, thereby greatly strengthening the continuity of Li-ion pathways in CLHEs and improving the kinetics of Li-ion transfer. The importance of an abundant solid–liquid interface for CLHEs was further verified by the enhanced electrochemical performance in LiFePO 4 /Li and LiNi 0.8 Co 0.1 Mn 0.1 O 2 /Li batteries from the generated interface. This work provides a clear understanding of the Li-ion transport pathway in CLHEs that serves as a basis to build a universal Li-ion transport model of CLHEs. [ABSTRACT FROM AUTHOR]

In article number 1805301, Yan‐Bing He and co‐workers report a low resistance integrated all‐solid‐state Li metal battery with excellent electrochemical performance. The battery structure applies polyethylene oxide with lithium bis(trifluoromethylsulphonyl)imide as both the binder of the cathode and matrix of the composite electrolyte embedded with Li7La3Zr2O12 nanowires. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium metal battery is the most promising next‐generation energy storage device. However, the low ionic conductivity of solid electrolytes and high interfacial impedance with electrode are the main factors to limit the development of all‐solid‐state batteries. In this work, a low resistance–integrated all‐solid‐state battery is designed with excellent electrochemical performance that applies the polyethylene oxide (PEO) with lithium bis(trifluoromethylsulphonyl)imide as both binder of cathode and matrix of composite electrolyte embedded with Li7La3Zr2O12 (LLZO) nanowires (PLLN). The PEO in cathode and PLLN are fused at high temperature to form an integrated all‐solid‐state battery structure, which effectively strengthens the interface compatibility and stability between cathode and PLLN to guarantee high efficient ion transportation during long cycling. The LLZO nanowires uniformly distributed in PLLN can increase the ionic conductivity and mechanical strength of composite electrolyte efficiently, which induces the uniform deposition of lithium metal, thereby suppressing the lithium dendrite growth. The Li symmetric cells using PLLN can stably cycle for 1000 h without short circuit at 60 °C. The integrated LiFePO4/PLLN/Li batteries show excellent cycling stability at both 60 and 45 °C. The study proposed a novel and robust battery structure with outstanding electrochemical properties. A low resistance–integrated all‐solid‐state Li metal battery with excellent electrochemical performance is designed. The structure not only guarantees high ionic conductivity and good mechanical properties to suppress lithium dendrite growth by using polyethylene oxide (PEO)/lithium bis(trifluoromethylsulphonyl)imide embedded with Li7La3Zr2O12 nanowire composite electrolyte, but also decreases the interfacial impedance by applying PEO in both electrolyte and cathode that can fuse during operation. [ABSTRACT FROM AUTHOR]

Abstract: Due to high energy density, low cost, and nontoxicity, lithium–sulfur (Li–S) batteries are considered as the most promising candidate to satisfy the requirement from the accelerated development of electric vehicles. However, Li–S batteries are subjected to lithium polysulfides (LiPSs) shuttling due to their high dissolution in liquid electrolyte, resulting in low columbic efficiency and poor cycling performance. Moreover, the Li metal as an indispensable anode of Li–S batteries shows serious safety issues derived from the lithium dendrite formation. The replacement of liquid electrolytes with solid‐state electrolytes (SSEs) has been recognized as a fundamental approach to effectively address above problems. In this review, the progress on applying various classes of SSEs including gel, solid‐state polymer, ceramic, and composite electrolytes to solve the issues of Li–S batteries is summarized. The specific capacity of Li–S batteries is effectively improved due to the suppression of LiPSs shuttling by SSEs, while the rate and cycling performance remain relatively poor owing to the limited ionic conductivity and high interfacial resistance. Designing smart electrode/electrolyte integrated architectures, enabling the high ionic transportation pathway and compatible electrode/electrolyte interface, may be an effective way to achieve high performance solid‐state Li–S batteries. [ABSTRACT FROM AUTHOR]

Graphene-based nanocomposites attract many attentions because of holding promise for many applications. In this work, multishelled NiO hollow spheres decorated by graphene nanosheets nanocomposite are successfully fabricated. The multishelled NiO microspheres are uniformly distributed on the surface of graphene, which is helpful for preventing aggregation of as-reduced graphene sheets. Furthermore, the NiO/graphene nanocomposite shows much higher electrochemical performance with a reversible capacity of 261.5 mAh g−1 at a current density of 200 mA g−1 after 100 cycles tripled compared with that of pristine multishelled NiO hollow spheres, implying the potential application in modern science and technology. [ABSTRACT FROM AUTHOR]