Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors. Issue 16 (7th March 2021)

• Record Type: Journal Article
• Authors: Lu, Ziheng; Yang, Ziwei; Li, Cheng; Wang, Kai; Han, Jinlong; Tong, Peifei; Li, Guoxiao; Vishnugopi, Bairav Sabarish; Mukherjee, Partha P.; Yang, Chunlei; Li, Wenjie
• Is Part Of: Advanced energy materials. Volume 11:Issue 16(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-03-07
• Subjects: conductive‐atomic force microscope -- critical current density -- lithium filament -- memristor -- solid‐state batteries; Energy harvesting -- Materials -- Periodicals; Energy conversion -- Materials -- Periodicals; Energy storage -- Materials -- Periodicals; Photovoltaics -- Periodicals; Fuel cells -- Periodicals; Thermoelectric materials -- Periodicals; 621.31
• DOI: 10.1002/aenm.202003811
• Languages: English
• ISSNs: 1614-6832

Abstract

Abstract: Dendrite penetration in ceramic lithium conductors severely constrains the development of solid‐state batteries (SSBs) while its nanoscale origin remains unelucidated. An in situ nanoscopic electrochemical characterization technique is developed based on conductive‐atomic force microscopy (c‐AFM) to reveal the local dendrite growth kinetics. Using Li7 La3 Zr2 O12 (LLZO) as a model system, significant local inhomogeneity is observed with a hundredfold decrease in the dendrite triggering bias at grain boundaries compared with that at grain interiors. The origin of the local weakening is assigned to the nanoscale variation of elastic modulus and lithium flux detouring. An ionic‐conductive polymeric homogenizing layer is designed which achieves a high critical current density of 1.8 mA cm –2 and a low interfacial resistance of 14 Ω cm 2 . Practical SSBs based on LiFePO4 cathodes can be stably cycled over 300 times. Beyond this, highly reversible electrochemical dendrite healing in LLZO is discovered using the c‐AFM electrode, based on which a model memristor with a high on/off ratio of ≈10 5 is demonstrated for >200 cycles. This work not only provides a novel tool to investigate and design interfaces in SSBs but also offers opportunities for solid electrolytes beyond energy applications. Abstract : Nanoscale dendrite growth kinetics in solid electrolytes are revealed by a high‐resolution in situ electrochemical characterization technique. Li + ‐flux homogenizing interfaces are designed for stable lithium plating. Solid‐state batteries with long cycle life are demonstrated. Electrochemical healing and memristive behavior of dendrites are revealed using nanoelectrodes. A memristor is designed and demonstrated using lithium solid electrolytes.