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Enabling High‐Energy Solid‐State Batteries with Stable Anode Interphase by the Use of Columnar Silicon Anodes
Author(s) -
Cangaz Sahin,
Hippauf Felix,
Reuter Florian Steffen,
Doerfler Susanne,
Abendroth Thomas,
Althues Holger,
Kaskel Stefan
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202001320
Subject(s) - materials science , anode , faraday efficiency , silicon , electrolyte , lithium (medication) , silicon monoxide , cathode , chemical engineering , nanotechnology , optoelectronics , electrode , electrical engineering , chemistry , engineering , endocrinology , medicine
All‐solid‐state batteries (ASSBs) with silicon anodes are promising candidates to overcome energy limitations of conventional lithium‐ion batteries. However, silicon undergoes severe volume changes during cycling leading to rapid degradation. In this study, a columnar silicon anode (col‐Si) fabricated by a scalable physical vapor deposition process (PVD) is integrated in all‐solid‐state batteries based on argyrodite‐type electrolyte (Li 6 PS 5 Cl, 3 mS cm −1 ) and Ni‐rich layered oxide cathodes (LiNi 0.9 Co 0.05 Mn 0.05 O 2 , NCM) with a high specific capacity (210 mAh g −1 ). The column structure exhibits a 1D breathing mechanism similar to lithium, which preserves the interface toward the electrolyte. Stable cycling is demonstrated for more than 100 cycles with a high coulombic efficiency (CE) of 99.7–99.9% in full cells with industrially relevant areal loadings of 3.5 mAh cm −2 , which is the highest value reported so far for ASSB full cells with silicon anodes. Impedance spectroscopy revealed that anode resistance is drastically reduced after first lithiation, which allows high charging currents of 0.9 mA cm −2 at room temperature without the occurrence of dendrites and short circuits. Finally, in‐operando monitoring of pouch cells gave valuable insights into the breathing behavior of the solid‐state cell.