TY - JOUR
T1 - Harnessing Metastable Byproducts
T2 - A Dual-Regulation Strategy for Intrinsically Stable High-Voltage Spinel Cathodes
AU - Wang, Qianchen
AU - Lv, Zhonghao
AU - Zhang, Zimo
AU - Zhang, Junkai
AU - Lu, Liyao
AU - Xin, Yuhang
AU - Wang, Yingshuai
AU - Gao, Hongcai
N1 - Publisher Copyright:
© 2026 American Chemical Society
PY - 2026/6/9
Y1 - 2026/6/9
N2 - Spinel LiNi0.5Mn1.5O4 (LNMO) suffers from Mn3+-induced degradation due to thermodynamic phase separation. Herein, we report the preincorporation of a LixNi1–xO (LNO) phase to regulate oxygen behavior through a dual-regulation strategy (interfacial charge modulation and kinetic facilitation of oxygen diffusion). Differential charge and Bader analyses confirm that the presence of LNO increases the covalency of the Mn–O bond and suppresses the release of oxygen. In situ EIS-DRT shows improved interfacial ion transport and suppressed side reactions. The optimized composite finally showed 54.2% less Mn3+, 76.2% higher oxygen vacancy energy, and 98.0% capacity retention over 300 cycles. This work will prove to be an overarching approach to stabilizing metastable cathodes by utilizing deleterious phases.
AB - Spinel LiNi0.5Mn1.5O4 (LNMO) suffers from Mn3+-induced degradation due to thermodynamic phase separation. Herein, we report the preincorporation of a LixNi1–xO (LNO) phase to regulate oxygen behavior through a dual-regulation strategy (interfacial charge modulation and kinetic facilitation of oxygen diffusion). Differential charge and Bader analyses confirm that the presence of LNO increases the covalency of the Mn–O bond and suppresses the release of oxygen. In situ EIS-DRT shows improved interfacial ion transport and suppressed side reactions. The optimized composite finally showed 54.2% less Mn3+, 76.2% higher oxygen vacancy energy, and 98.0% capacity retention over 300 cycles. This work will prove to be an overarching approach to stabilizing metastable cathodes by utilizing deleterious phases.
UR - https://www.scopus.com/pages/publications/105041333760
U2 - 10.1021/acs.chemmater.6c00887
DO - 10.1021/acs.chemmater.6c00887
M3 - Article
AN - SCOPUS:105041333760
SN - 0897-4756
VL - 38
SP - 5744
EP - 5752
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 11
ER -