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Glassy Na-ion solid-state electrolytes (GNSSEs) are an important group of amorphous SSEs. However, the insufficient ionic conductivity of state-of-the-art GNSSEs at room temperature lessens their promise in the development of all-solid-state Na-ion batteries (ASSNIBs) with high energy density and improved safety. Here we report the discovery of a new sodium superionic glass, 0.5Na2 O2 -TaCl5 (NTOC), based on dual-anion sublattice of oxychlorides. The unique local structures with abundant bridging and non-bridging oxygen atoms contributes to a highly disordered Na-ion distribution as well as low Na+ migration barrier within NTOC, enabling an ultrahigh ionic conductivity of 4.62 mS cm-1 at 25 °C (more than 20 times higher than those of previously reported GNSSEs). Moreover, the excellent formability of glassy NTOC electrolyte and its high electrochemical oxidative stability ensure a favourable electrolyte-electrode interface, contributing to superior cycling stability of ASSNIBs for over 500 cycles at room temperature. The discovery of glassy NTOC electrolyte would reignite research enthusiasm in superionic glassy SSEs based on multi-anion chemistry.

Amorphous solid‐state electrolytes (SSEs) play a pivotal role as fundamental components within all‐solid‐state lithium batteries, yet their understanding lags behind that of crystalline materials. In this work, a novel amorphous SSE 5Li2S‐3SiS2 (mol %) with a high ionic conductivity of 1.2 mS cm−1 is first reported. The silicon and sulfur atoms in the edge‐sharing Si2S64− are less attracted to lithium compared to the SiS44− anion, which is expected to facilitate the lithium ions conduction in SSEs. More importantly, the relationship between the material properties and local structure in the amorphous thiosilicate SSEs is revealed, particularly highlighting the desirable edge‐sharing local structure. The Si2S64− presents better stability with Li metal. This work offers an important guideline in the development of anion frameworks in amorphous sulfide SSEs for high‐performance all‐solid‐state lithium metal batteries. [ABSTRACT FROM AUTHOR]

All-solid-state lithium-sulfur batteries offer a compelling opportunity for next-generation energy storage, due to their high theoretical energy density, low cost, and improved safety. However, their widespread adoption is hindered by an inadequate understanding of their discharge products. Using X-ray absorption spectroscopy and time-of-flight secondary ion mass spectrometry, we reveal that the discharge product of all-solid-state lithium-sulfur batteries is not solely composed of Li2S, but rather consists of a mixture of Li2S and Li2S2. Employing this insight, we propose an integrated strategy that: (1) manipulates the lower cutoff potential to promote a Li2S2-dominant discharge product and (2) incorporates a trace amount of solid-state catalyst (LiI) into the S composite electrode. This approach leads to all-solid-state cells with a Li-In alloy negative electrode that deliver a reversible capacity of 979.6 mAh g−1 for 1500 cycles at 2.0 A g−1 at 25 °C. Our findings provide crucial insights into the discharge products of all-solid-state lithium-sulfur batteries and may offer a feasible approach to enhance their overall performance. All-solid-state lithium sulfur batteries may avoid some of the drawbacks of their liquid electrolyte counterparts. Here, the authors elucidate the composition of discharge products in all-solid-state cells using spectroscopic techniques and propose a strategy to control the discharge product. [ABSTRACT FROM AUTHOR]

Due to high ionic conductivity and low cost, Li1.4Al0.4Ti1.6(PO4)3 (LATP) has emerged as a promising solid‐state electrolyte for next‐generation lithium (Li) metal solid‐state batterie with high safety performance and energy density. However, the extremely high impedance and surface instability of LATP with Li metal retard its practical application. Herein, a novel method is proposed to construct an ultrathin ZnO layer that is tightly coated on the LATP pellets, surface (ZnO@LATP) via magnetron sputtering, which in situ reacts with Li to form a low electronic conductivity and multifunctional solid electrolyte interphase (SEI). The formed SEI can not only effectively lower the interfacial resistance, but also overcome the side reactions of LATP with the Li metal anode and suppress the Li dendrite growth. Specifically, the interface resistance decreases from 80 554 to 353 Ω and the overpotential reduces from 1 V to 20 mV. As a result, the Li/ZnO@LATP@ZnO/Li symmetric batteries can stably cycle for more than 2000 h without short circuit at 0.05 mA cm−2 and Li/ZnO@LATP/LiFePO4 batteries show excellent cycle stability for 200 cycles at 0.1 C. This work highlights the significance of multifunctional interphase between LATP and Li metal for improvement of interfacial impedance and instability. [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]

The evolution of inorganic solid electrolytes has revolutionized the field of sustainable organic cathode materials, particularly by addressing the dissolution problems in traditional liquid electrolytes. However, current sulfide-based all-solid-state lithium-organic batteries still face challenges such as high working temperatures, high costs, and low voltages. Here, we design an all-solid-state lithium battery based on a cost-effective organic cathode material phenanthrenequinone (PQ) and a halide solid electrolyte Li 2 ZrCl 6 . Thanks to the good compatibility between PQ and Li 2 ZrCl 6 , the PQ cathode achieved a high specific capacity of 248 mAh g -1 (96 % of the theoretical capacity), a high average discharge voltage of 2.74 V (vs. Li + /Li), and a good capacity retention of 95 % after 100 cycles at room temperature (25 °C). Furthermore, the interactions between the high-voltage carbonyl PQ cathode and both sulfide and halide solid electrolytes, as well as the redox mechanism of the PQ cathode in all-solid-state batteries, were carefully studied by a variety of advanced characterizations. We believe such a design and the corresponding investigations into the underlying chemistry give insights for the further development of practical all-solid-state lithium-organic batteries., (© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Glassy Na-ion solid-state electrolytes (GNSSEs) are an important group of amorphous SSEs. However, the insufficient ionic conductivity of state-of-the-art GNSSEs at room temperature lessens their promise in the development of all-solid-state Na-ion batteries (ASSNIBs) with high energy density and improved safety. Here we report the discovery of a new sodium superionic glass, 0.5Na 2 O 2 -TaCl 5 (NTOC), based on dual-anion sublattice of oxychlorides. The unique local structures with abundant bridging and non-bridging oxygen atoms contributes to a highly disordered Na-ion distribution as well as low Na + migration barrier within NTOC, enabling an ultrahigh ionic conductivity of 4.62 mS cm -1 at 25 °C (more than 20 times higher than those of previously reported GNSSEs). Moreover, the excellent formability of glassy NTOC electrolyte and its high electrochemical oxidative stability ensure a favourable electrolyte-electrode interface, contributing to superior cycling stability of ASSNIBs for over 500 cycles at room temperature. The discovery of glassy NTOC electrolyte would reignite research enthusiasm in superionic glassy SSEs based on multi-anion chemistry., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Insertion-type compounds based on oxides and sulfides have been widely identified and well-studied as cathode materials in lithium-ion batteries. However, halides have rarely been used due to their high solubility in organic liquid electrolytes. Here, we reveal the insertion electrochemistry of VX 3 (X=Cl, Br, I) by introducing a compatible halide solid-state electrolyte with a wide electrochemical stability window. X-ray absorption near-edge structure analyses reveal a two-step lithiation process and the structural transition of typical VCl 3 . Fast Li + insertion/extraction in the layered VX 3 active materials and favorable interface guaranteed by the compatible electrode-electrolyte design enables high rate capability and stable operation of all-solid-state Li-VX 3 batteries. The findings from this study will contribute to developing intercalation insertion electrochemistry of halide materials and exploring novel electrode materials in viable energy storage systems., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)