Garnet-type solid-state electrolytes have attracted extensive attention due to their high ionic conductivity, approaching 1 mS cm, excellent environmental stability, and wide electrochemical stability window, from lithium metal to ∼6 V. However, to date, there has been little success in the development of high-performance solid-state batteries using these exceptional materials, the major challenge being the high solid-solid interfacial impedance between the garnet electrolyte and electrode materials. In this work, we effectively address the large interfacial impedance between a lithium metal anode and the garnet electrolyte using ultrathin aluminium oxide (AlO) by atomic layer deposition. LiLaCaZrNbO (LLCZN) is the garnet composition of choice in this work due to its reduced sintering temperature and increased lithium ion conductivity. A significant decrease of interfacial impedance, from 1,710 Ω cm to 1 Ω cm, was observed at room temperature, effectively negating the lithium metal/garnet interfacial impedance. Experimental and computational results reveal that the oxide coating enables wetting of metallic lithium in contact with the garnet electrolyte surface and the lithiated-alumina interface allows effective lithium ion transport between the lithium metal anode and garnet electrolyte. We also demonstrate a working cell with a lithium metal anode, garnet electrolyte and a high-voltage cathode by applying the newly developed interface chemistry.

Strategy to change the wettability of the solid-state electrolyte against Li and reduce interface resistance.

Solid-state electrolytes are known for nonflammability, dendrite blocking, and stability over large potential windows. Garnet-based solid-state electrolytes have attracted much attention for their high ionic conductivities and stability with lithium metal anodes. However, high-interface resistance with lithium anodes hinders their application to lithium metal batteries. Here, we demonstrate an ultrathin, conformal ZnO surface coating by atomic layer deposition for improved wettability of garnet solid-state electrolytes to molten lithium that significantly decreases the interface resistance to as low as ∼20 Ω·cm. The ZnO coating demonstrates a high reactivity with lithium metal, which is systematically characterized. As a proof-of-concept, we successfully infiltrated lithium metal into porous garnet electrolyte, which can potentially serve as a self-supported lithium metal composite anode having both high ionic and electrical conductivity for solid-state lithium metal batteries. The facile surface treatment method offers a simple strategy to solve the interface problem in solid-state lithium metal batteries with garnet solid electrolytes.

All-solid-state Li-batteries using solid-state electrolytes (SSEs) offer enhanced safety over conventional Li-ion batteries with organic liquid electrolytes due to the nonflammable nature of SSEs. The superior mechanical strength of SSEs can also protect against Li dendrite penetration, which enables the use of the highest specific capacity (3861 mAh/g) and lowest redox potential (-3.04 V vs standard hydrogen electrode) anode: Li metal. However, contact between the Li metal and SSEs presents a major challenge, where a large polarization occurs at the Li metal/SSE interface. Here, the chemical properties of a promising oxide-based SSE (garnet) changed from "super-lithiophobicity" to "super-lithiophilicity" through an ultrathin coating of amorphous Si deposited by plasma-enhanced chemical vapor deposition (PECVD). The wettability transition is due to the reaction between Li and Si and the in situ formation of lithiated Si. As a result, symmetric cells composed of a Si-coated garnet-structured SSE and Li metal electrodes exhibited much smaller impedance and excellent stability upon plating/stripping cycles compared to cells using bare garnet SSE. Specifically, the interfacial resistance between Li and garnet dramatically decreased from 925 to 127 Ω cm(2) when lithiated Si was formed on the garnet. Our discovery of switchable lithiophobic-lithiophilic surfaces to improve the Li metal/SSE interface opens opportunities for improving many other SSEs.

A solid electrolyte framework with porous and dense layers for high-energy and safe Li-metal batteries.

Using solar energy to generate steam is a clean and sustainable approach to addressing the issue of water shortage. The current challenge for solar steam generation is to develop easy-to-manufacture and scalable methods which can convert solar irradiation into exploitable thermal energy with high efficiency. Although various material and structure designs have been reported, high efficiency in solar steam generation usually can be achieved only at concentrated solar illumination. For the first time, 3D printing to construct an all-in-one evaporator with a concave structure for high-efficiency solar steam generation under 1 sun illumination is used. The solar-steam-generation device has a high porosity (97.3%) and efficient broadband solar absorption (>97%). The 3D-printed porous evaporator with intrinsic low thermal conductivity enables heat localization and effectively alleviates thermal dissipation to the bulk water. As a result, the 3D-printed evaporator has a high solar steam efficiency of 85.6% under 1 sun illumination (1 kW m ), which is among the best compared with other reported evaporators. The all-in-one structure design using the advanced 3D printing fabrication technique offers a new approach to solar energy harvesting for high-efficiency steam generation.

Lithium dendrite (filament) propagation through ceramic electrolytes, leading to short-circuits at high rates of charge, is one of the greatest barriers to realising high energy density all-solidstate lithium anode batteries. Utilising in-situ X-ray computed tomography coupled with spatially mapped X-ray diffraction, the propagation of cracks and the propagation of lithium dendrites through the solid electrolyte have been tracked in a Li/Li6PS5Cl/Li cell as a function of the charge passed. On plating, cracking initiates with spallation, conical "pothole"-like cracks that form in the ceramic electrolyte near the surface with the plated electrode. The spallations form predominantly at the lithium electrode edges where local fields are high. Transverse cracks then propagate from the spallations across the electrolyte from the plated to the stripped electrode. Lithium ingress drives the propagation of the spallation and transverse cracks by widening the crack from the rear, i.e. the crack front propagates ahead of the Li. As a result, cracks traverse the entire electrolyte before the Li arrives at the other electrode and therefore before a short-circuit occurs.

Space cooling is a predominant part of energy consumption in people's daily life. Although cooling the whole building is an effective way to provide personal comfort in hot weather, it is energy-consuming and high-cost. Personal cooling technology, being able to provide personal thermal comfort by directing local heat to the thermally regulated environment, has been regarded as one of the most promising technologies for cooling energy and cost savings. Here, we demonstrate a personal thermal regulated textile using thermally conductive and highly aligned boron nitride (BN)/poly(vinyl alcohol) (PVA) composite (denoted as a-BN/PVA) fibers to improve the thermal transport properties of textiles for personal cooling. The a-BN/PVA composite fibers are fabricated through a fast and scalable three-dimensional (3D) printing method. Uniform dispersion and high alignment of BN nanosheets (BNNSs) can be achieved during the processing of fiber fabrication, leading to a combination of high mechanical strength (355 MPa) and favorable heat dispersion. Due to the improved thermal transport property imparted by the thermally conductive and highly aligned BNNSs, better cooling effect (55% improvement over the commercial cotton fiber) can be realized in the a-BN/PVA textile. The wearable a-BN/PVA textiles containing the 3D-printed a-BN/PVA fibers offer a promising selection for meeting the personal cooling requirement, which can significantly reduce the energy consumption and cost for cooling the whole building.