Building a Better Li‐Garnet Solid Electrolyte/Metallic Li Interface with Antimony

Abstract

The deployment of Li‐garnet Li7La3Zr2O12 (LLZO) solid‐state electrolytes in solid‐state batteries is severely hampered by their poor wettability with metallic Li. In this work, Sb is presented as a compelling interfacial layer allowing superior wetting of Li onto a LLZO surface, resulting in a remarkably low Li/LLZO interfacial resistance of 4.1(1) Ω cm2. An atomistic insight into Sb‐coated LLZO interface using soft and hard X‐ray photoelectron spectroscopy and focused ion beam time‐of‐flight secondary ion mass spectrometry shows the formation of a Li‐Sb alloy as an interlayer. It is determined that the Li/Sb‐coated LLZO/Li symmetrical cells exhibit a high critical current density of up to 0.64 mA cm−2 and low overpotentials of 40–50 mV at a current density of 0.2 mA cm−2 without applying external pressure. The electrochemical performance of Sb coated‐LLZO pellets is also assessed with an intercalation‐type V2O5 cathode. Li/Sb‐coated‐LLZO/V2O5 full cells deliver stable capacities of around 0.45 mAh cm−2, with a peak current density of 0.3 mA cm−2.

Spiers Memorial Lecture: prospects for photoelectron spectroscopy

“…116 In particular, HAXPES has proved strikingly powerful in locating and characterising layers and buried interfaces, 117 for example in devices (such as prototype metal-oxide-semiconductor eld effect transistor devices, https://doi.org/10.1039/D1FD00110H 118 and spintronic materials 119 ) and interphases, for example the solid electrolyte interphase in battery materials. [120][121][122] In both cases, there are signicant advantages in making measurements in a more realistic environment in a working device or cell, moving towards in operando conditions. Although much of this work has been carried out with synchrotron sources, the new generation of lab-based sources make this work viable in the laboratory.…”

“…In the case of battery materials, the difficulties in approaching operando conditions are perhaps more signicant, and much of the initial work was carried out with ex situ electrochemical cycling, with the material subsequently recovered from the cells for examination. 120,121 More recently, however, it has become possible to obtain HAXPES from prototype cells during charging and discharging in situ inside the UHV chamber. An example, from BL28XU at SPring-8, is the observation of reversible changes in the Co 2p and O 1s spectra during in situ cycling of a LiCoO 2 thin lm cell.…”

Room-temperature–low-pressure-operating high-energy lithium metal batteries employing garnet-type solid electrolytes and anode interlayers

“…To the best of our knowledge, these commercial-level performances at 25°C is the rst reported in Li metal batteries employing a solid oxide electrolyte, as described in Fig. 7 [31][32][33][34][35][36][37][38][39][40][41][42][43][44][45][46] .…”

Design of a Self‐Powered System by Wind‐Driven Triboelectric Nanogenerator Based on 0.94(Bi0.5Na0.5)TiO3–0.06Ba(Zr0.25Ti0.75)O3/Polyvinylidene Fluoride (BNT–BZT/PVDF) Composites

“…[36,37] For solid electrolytes, garnet-type solid electrolytes, particularly ceramic Li 7 La 3 Zr 2 O 12 (LLZO), have been extensively studied because of their high ionic conductivity and excellent thermal property. [38][39][40] However, the high interface resistance between LLZO and the solid electrode normally leads to inferior battery performance. [41,42] Besides, the hard and brittle drawbacks of ceramic LLZO material also make it difficult to prepare flakes that are suitable for electrolytes, thus preventing its application in solid-state electrolytes.…”