TY - JOUR
T1 - Molten-salt-mediated crystal facet engineering for high-performance single-crystal nickel-rich cathode materials in lithium-ion batteries
AU - Zhang, Hongyun
AU - Dong, Jinyang
AU - Lu, Yun
AU - Liu, Yun
AU - Hao, Jianan
AU - Li, Ning
AU - Chen, Gang
AU - Huang, Qing
AU - Su, Yuefeng
AU - Wu, Feng
AU - Chen, Lai
N1 - Publisher Copyright:
© 2025 Elsevier Ltd
PY - 2025/9
Y1 - 2025/9
N2 - Nickel-rich layered oxide cathodes are promising candidates for lithium-ion batteries due to high energy density and cost efficiency. However, their utilization is constrained by structural instability, slow lithium-ion transport, and capacity degradation under high cut-off voltage cycling. This investigation employed a molten-salt-mediated synthesis strategy to fabricate single-crystal nickel-rich layered oxide cathodes (SCNCMs) with controlled crystallographic plane exposure. Anion-regulated crystal growth adjusted the (104) plane exposure to enhance Li+ ion diffusion and mitigate the formation of oxygen vacancies. Theoretical calculations and experimental results confirmed that increased (104) plane exposure improved electrochemical performance, mechanical strength, and cycling stability. Pouch-type full-cell tests demonstrated that the SCNCM prepared using KBr (SC-B) with a higher (104) exposure exhibited exceptional long-term cycling stability compared to that of the pristine SCNCM prepared using traditional KCl (SC-C). After 600 cycles, SC-B retained 82.11 % of its initial capacity, whereas SC-C lost over 65 %. SC-B also demonstrated superior rate capability under high-power conditions. Theoretical modeling revealed that facet modulation is crucial for lithium-ion distribution and stress evolution, highlighting the importance of crystallographic control on the cathode performance. These findings provide a framework for high-performance single-crystal cathodes and insights into the structural optimization of next-generation lithium-ion battery materials.
AB - Nickel-rich layered oxide cathodes are promising candidates for lithium-ion batteries due to high energy density and cost efficiency. However, their utilization is constrained by structural instability, slow lithium-ion transport, and capacity degradation under high cut-off voltage cycling. This investigation employed a molten-salt-mediated synthesis strategy to fabricate single-crystal nickel-rich layered oxide cathodes (SCNCMs) with controlled crystallographic plane exposure. Anion-regulated crystal growth adjusted the (104) plane exposure to enhance Li+ ion diffusion and mitigate the formation of oxygen vacancies. Theoretical calculations and experimental results confirmed that increased (104) plane exposure improved electrochemical performance, mechanical strength, and cycling stability. Pouch-type full-cell tests demonstrated that the SCNCM prepared using KBr (SC-B) with a higher (104) exposure exhibited exceptional long-term cycling stability compared to that of the pristine SCNCM prepared using traditional KCl (SC-C). After 600 cycles, SC-B retained 82.11 % of its initial capacity, whereas SC-C lost over 65 %. SC-B also demonstrated superior rate capability under high-power conditions. Theoretical modeling revealed that facet modulation is crucial for lithium-ion distribution and stress evolution, highlighting the importance of crystallographic control on the cathode performance. These findings provide a framework for high-performance single-crystal cathodes and insights into the structural optimization of next-generation lithium-ion battery materials.
KW - Facet engineering
KW - Lithium-ion batteries
KW - Molten salt synthesis
KW - Nickel-rich cathodes
KW - Single-crystal
UR - http://www.scopus.com/inward/record.url?scp=105006711217&partnerID=8YFLogxK
U2 - 10.1016/j.nanoen.2025.111177
DO - 10.1016/j.nanoen.2025.111177
M3 - Article
AN - SCOPUS:105006711217
SN - 2211-2855
VL - 142
JO - Nano Energy
JF - Nano Energy
M1 - 111177
ER -