TY  - JOUR
AU  - Huang, Zhongyuan
AU  - Chen, Ziwei
AU  - Yang, Maolin
AU  - Chu, Mihai
AU  - Li, Zenan
AU  - Deng, Sihao
AU  - He, Lunhua
AU  - Jin, Lei
AU  - Dunin-Borkowski, Rafal E.
AU  - Wang, Rui
AU  - Wang, Jun
AU  - Yang, Tingting
AU  - Xiao, Yinguo
TI  - Insights into the defect-driven heterogeneous structural evolution of Ni-rich layered cathodes in lithium-ion batteries
JO  - Energy & environmental science
VL  - 17
IS  - 16
SN  - 1754-5692
CY  - Cambridge
PB  - RSC Publ.
M1  - FZJ-2024-07252
SP  - 5876 - 5891
PY  - 2024
AB  - Recently, considerable efforts have been made in research and development to improve Ni-rich lithium-ion batteries to meet the demands of vehicles and grid-level large-scale energy storage. The development of next-generation high-performance lithium-ion batteries requires a comprehensive understanding of the underlying electrochemical mechanisms associated with their structural evolution. In this work, advanced operando neutron diffraction and four-dimensional scanning transmission electron microscopy techniques were applied to clarify the structural evolution of electrodes in two distinct full cells with identical LiNi0.8Co0.1Mn0.1O2 cathodes but different anode counterparts. It is found that both cathodes in the two cells exhibit non-intrinsic two-phase-like behavior at the early charge stage, indicating selective Li+ extraction from cathodes. But the heterogeneous evolution of cathodes is inhibited with a graphite–silicon blended anode compared to that with a graphite anode due to differences in the delithiation rate. Moreover, it is revealed that the formation of heterogeneous structures is driven by the distribution of defects including Li/Ni disordering and microcracks, which should be inhibited by assembling an appropriate anode to avoid potential threats to cell performance. The present work unveils the origin of inhomogeneity in Ni-rich lithium-ion batteries and highlights the significance of kinetics control in electrodes for batteries with higher capacity and longer life.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001272050500001
DO  - DOI:10.1039/D4EE01777C
UR  - https://juser.fz-juelich.de/record/1034486
ER  -