Enabling High-Energy Solid-State Batteries with Stable Anode Interphase by the Use of Columnar Silicon Anodes

被引:152
作者
Cangaz, Sahin [1 ,2 ]
Hippauf, Felix [2 ]
Reuter, Florian Steffen [1 ,2 ]
Doerfler, Susanne [2 ]
Abendroth, Thomas [2 ]
Althues, Holger [2 ]
Kaskel, Stefan [1 ,2 ]
机构
[1] Tech Univ Dresden, Chair Inorgan Chem 1, Bergstr 66, D-01069 Dresden, Germany
[2] Fraunhofer Inst Mat & Beam Technol IWS, Winterbergstr 28, D-01277 Dresden, Germany
关键词
all-solid-state batteries; columnar silicon anodes; in situ investigation; thiophosphate solid electrolytes; volumetric energy density; LITHIUM-ION BATTERIES; SI FILM ANODE; LI-ION; FLUOROETHYLENE CARBONATE; ELECTROLYTE ADDITIVES; VINYLENE CARBONATE; AMORPHOUS-SILICON; PERFORMANCE; COMPOSITE; CAPACITY;
D O I
10.1002/aenm.202001320
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 (Li6PS5Cl, 3 mS cm(-1)) and Ni-rich layered oxide cathodes (LiNi0.9Co0.05Mn0.05O2, 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.
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页数:10
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