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Rectifying interphases for preventing Li dendrite propagation in solid-state electrolytes

Yao, Xuhui; Lu, Xuekun; Zhou, Yundong; Šamořil, Tomáš; Bi, Jinxin; Masteghin, Mateus G; Zhang, Huixing; ... Zhao, Yunlong; + view all (2023) Rectifying interphases for preventing Li dendrite propagation in solid-state electrolytes. Energy & Environmental Science 10.1039/d2ee04006a. (In press). Green open access

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Abstract

Solid-state electrolytes have emerged as the grail for safe and energy-dense Li metal batteries but still face significant challenges of Li dendrite propagation and interfacial incompatibility. In this work, an interface engineering approach is applied to introduce an electronic rectifying interphase between the solid-state electrolyte and Li metal anode. The rectifying behaviour restrains electron infiltration into the electrolyte, resulting in effective dendrite reduction. This interphase consists of a p-Si/n-TiO2 junction and an external Al layer, created using a multi-step sputter deposition technique on the surface of garnet pellets. The electronic rectifying behaviour is investigated via the asymmetric I-V responses of on-chip devices and further confirmed via the one-order of magnitude lower current response by electronic conductivity measurements on the pellets. The Al layer contributes to interface compatibility, which is verified from the lithiophilic surface and reduced interfacial impedance. Electrochemical measurements via Li symmetric cells show a significantly improved lifetime from dozens of hours to over two months. The reduction of the Li dendrite propagation behaviour is observed through 3D reconstructed morphologies of the solid-state electrolyte by X-ray computed tomography.

Type: Article
Title: Rectifying interphases for preventing Li dendrite propagation in solid-state electrolytes
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d2ee04006a
Publisher version: http://doi.org/10.1039/d2ee04006a
Language: English
Additional information: Open Access Article. Published on 21 March 2023. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (https://creativecommons.org/licenses/by/3.0/).
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10168886
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