TY - JOUR
T1 - Interface Modeling via Tailored Energy Band Alignment
T2 - Toward Electrochemically Stabilized All-Solid-State Li-Metal Batteries
AU - Kim, Heebae
AU - Im, Changik
AU - Ryu, Seokgyu
AU - Gong, Yong Jun
AU - Cho, Jinil
AU - Pyo, Seonmi
AU - Yun, Heejun
AU - Lee, Jeewon
AU - Yoo, Jeeyoung
AU - Kim, Youn Sang
N1 - Publisher Copyright:
© 2021 Wiley-VCH GmbH
PY - 2022/2/23
Y1 - 2022/2/23
N2 - Interfacial instability between Li-metal anode (LMA) and inorganic solid-state electrolyte (SSE) is a critical issue in all-solid-state Li-metal batteries (ASSLBs). Previous studies have focused on interface modification methodology to achieve long-term cycling stability in ASSLBs. However, strategy establishment without an in-depth understanding of the LMA–SSE interface is limited to a phenomenological solution. Also, the fact that rechargeable batteries are operated by behavior of charges inside electric field is frequently overlooked. Here, it is demonstrated for the first time that interface modeling based on energy band theory does effectively overcome the intrinsic vulnerability of SSE to LMA. The interfacial deterioration, due to undesirable electron transport from LMA to the SSE surface, is precluded by a titanium compound self-induced interlayer (TSI), which forms an interfacial energy barrier. The Li symmetric cell with a TSI successfully maintains its constant overpotential over 1000 cycles and the significantly reduced impedance, whereas the cell having no interface modification exhibits erratic voltage profiles and is easily failed by repetitive charge–discharge process. This newly introduced approach is an informative tool to substantially reinforce the fundamental understanding of interfacial phenomena in all-solid-state batteries. Furthermore, rigorous stability requirements of automotive applications are expected to be fulfilled by the innovative interface modification.
AB - Interfacial instability between Li-metal anode (LMA) and inorganic solid-state electrolyte (SSE) is a critical issue in all-solid-state Li-metal batteries (ASSLBs). Previous studies have focused on interface modification methodology to achieve long-term cycling stability in ASSLBs. However, strategy establishment without an in-depth understanding of the LMA–SSE interface is limited to a phenomenological solution. Also, the fact that rechargeable batteries are operated by behavior of charges inside electric field is frequently overlooked. Here, it is demonstrated for the first time that interface modeling based on energy band theory does effectively overcome the intrinsic vulnerability of SSE to LMA. The interfacial deterioration, due to undesirable electron transport from LMA to the SSE surface, is precluded by a titanium compound self-induced interlayer (TSI), which forms an interfacial energy barrier. The Li symmetric cell with a TSI successfully maintains its constant overpotential over 1000 cycles and the significantly reduced impedance, whereas the cell having no interface modification exhibits erratic voltage profiles and is easily failed by repetitive charge–discharge process. This newly introduced approach is an informative tool to substantially reinforce the fundamental understanding of interfacial phenomena in all-solid-state batteries. Furthermore, rigorous stability requirements of automotive applications are expected to be fulfilled by the innovative interface modification.
KW - Li-metal anodes
KW - all-solid-state batteries
KW - solid-state electrolytes
KW - stable interfaces
UR - http://www.scopus.com/inward/record.url?scp=85119112641&partnerID=8YFLogxK
U2 - 10.1002/adfm.202107555
DO - 10.1002/adfm.202107555
M3 - Article
AN - SCOPUS:85119112641
SN - 1616-301X
VL - 32
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 9
M1 - 2107555
ER -