TY - JOUR
T1 - Molecular design through d-orbital induced electron redistribution tailors Li+coordination and cathode interfacial chemistry towards stable ultra-rich nickel Li batteries
AU - Huang, Yuanyuan
AU - Wu, Junru
AU - Zhao, Yun
AU - Yang, Shu
AU - Wang, Xianshu
AU - Cao, Yuanpeng
AU - Zhou, Zhuo
AU - Yin, Xiangshao
AU - Luo, Liang
AU - Pan, Zhenghui
AU - Duan, Jianguo
AU - Wang, Ding
AU - Dong, Peng
AU - He, Pan
AU - Zhang, Yingjie
AU - Li, Baohua
N1 - Publisher Copyright:
© 2026 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
PY - 2026/5
Y1 - 2026/5
N2 - Weakly solvation chemistry is an effective approach to stabilize LiNixCoyMn1-x-yO2 (x ≥ 0.8) cathode for high energy density lithium-ion batteries (LIBs). Herein, we propose a d-orbital-induced electron redistribution-tailored solvation strategy that not only weakens Li+coordination and promotes anion-involved solvation, but also leverages coordination groups to actively participate in interfacial reactions, thereby forming multiphase hybrid cathode electrolyte interphase (CEI) to enhance LiNi0.98Co0.02O2 battery performance. This strategy originates sulfur (S) atom utilizes its empty 3d-orbitals to induce the redistribution of the lone electron pair on the coordinated oxygen (O) atoms inside the 1,3-propylene sulfite (PSi), derived from ethylene carbonate (EC) after carbocycle regulation and S atom substitution. Computational and spectroscopic analyses confirm the reduced electron density on the sulfinyl oxygen (OSO) of PSi. Sulfinyl oxygen groups together with anion form a multiphase stabilized CEI. Consequently, PSi-based electrolyte enhances the electrochemical performance of LiNi0.98Co0.02O2 cells, delivering 83.67 % capacity retention over 300 cycles at 0.5 C and 158.44 mAh/g at 5 C in half cells, and 83.44 % capacity retention after 500 cycles in full cells, and 82.0 % capacity retention over 120 cycles in 1.68 Ah pouch cells. These results demonstrate a molecular-level electrolyte design principle for better interface chemistry and LIBs.
AB - Weakly solvation chemistry is an effective approach to stabilize LiNixCoyMn1-x-yO2 (x ≥ 0.8) cathode for high energy density lithium-ion batteries (LIBs). Herein, we propose a d-orbital-induced electron redistribution-tailored solvation strategy that not only weakens Li+coordination and promotes anion-involved solvation, but also leverages coordination groups to actively participate in interfacial reactions, thereby forming multiphase hybrid cathode electrolyte interphase (CEI) to enhance LiNi0.98Co0.02O2 battery performance. This strategy originates sulfur (S) atom utilizes its empty 3d-orbitals to induce the redistribution of the lone electron pair on the coordinated oxygen (O) atoms inside the 1,3-propylene sulfite (PSi), derived from ethylene carbonate (EC) after carbocycle regulation and S atom substitution. Computational and spectroscopic analyses confirm the reduced electron density on the sulfinyl oxygen (OSO) of PSi. Sulfinyl oxygen groups together with anion form a multiphase stabilized CEI. Consequently, PSi-based electrolyte enhances the electrochemical performance of LiNi0.98Co0.02O2 cells, delivering 83.67 % capacity retention over 300 cycles at 0.5 C and 158.44 mAh/g at 5 C in half cells, and 83.44 % capacity retention after 500 cycles in full cells, and 82.0 % capacity retention over 120 cycles in 1.68 Ah pouch cells. These results demonstrate a molecular-level electrolyte design principle for better interface chemistry and LIBs.
KW - 1,3-propylene sulfite
KW - Cathode electrolyte interphase
KW - Electron redistribution
KW - Lithium-ion batteries
KW - Ultrahigh nickel layered oxide cathode
UR - https://www.scopus.com/pages/publications/105033148970
U2 - 10.1016/j.nanoen.2026.111817
DO - 10.1016/j.nanoen.2026.111817
M3 - Article
AN - SCOPUS:105033148970
SN - 2211-2855
VL - 151
JO - Nano Energy
JF - Nano Energy
M1 - 111817
ER -