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In Situ Neutron Powder Diffraction Using Custom-made Lithium-ion Batteries
Published on: November 10, 2014
Ternary Dimension-Synergistic Conductive Architecture Enabling High-Rate, Low-Temperature and Extended-Cycling
Zhongyuan Li1, Hongda Yang1, Minhu Xu1
1Electric Power Research Institute, State Grid Heilongjiang Electric Power Co., Ltd., Harbin 150030, China.
Abstract:
The severe performance degradation of lithium-ion batteries at low temperatures limits their applications in extreme environments. Herein, we report the development of a low-temperature-capable 2.5 Ah 18650 cylindrical battery employing a LiNi0.8Co0.15Al0.05O2 cathode with optimized conductive additive formulations. The ternary conductive architecture is rationally designed based on dimensional complementarity: a zero-dimensional Super P (SP) nanoparticle ensures percolation through point-to-point contacts, a one-dimensional multi-walled carbon nanotube (MWCNT) establishes long-range electron highways via line-to-point bridging, and a two-dimensional graphene nanoplatelet (GNP) provides face-to-point encapsulation of active particles, mechanically buffering volume expansion and suppressing interfacial degradation. This hierarchical point-line-plane network generates redundant electron transport pathways while steric hindrance effects mitigate aggregation of each component. Through systematic comparative investigation of GNP/MWCNT/SP ternary and MWCNT/SP binary conductive systems, we elucidate the distinct roles of low-dimensional nanocarbons in electrochemical performance enhancement. Film resistivity measurements reveal that the ternary system achieves a 67% reduction in cathode resistivity (to 9.1 Ω·cm at 20 °C) compared to conventional SP (27.5 Ω·cm), outperforming previously reported binary nanocarbon systems for high-nickel cathodes (typically 40-55% reduction at comparable loadings). This enhancement is achieved at a constant total conductive additive loading of 2.5 wt%, demonstrating that dimensional optimization rather than quantity increase governs electrical transport properties. Electrochemical evaluations demonstrate that the fabricated 18650 cells deliver exceptional rate capability (10C continuous and 20C pulse discharge) and remarkable low-temperature performance (76.8% capacity retention at -40 °C under 1C). Notably, while both conductive formulations exhibit comparable rate performan ce and temperature adaptability, the ternary GNP/MWCNT/SP system demonstrates significant superiority in cycling stability, achieving 94.9% capacity retention after 1000 cycles at ambient temperature versus inferior retention for the binary counterpart. Electrochemical impedance spectroscopy analyses indicate reduced polarization and enhanced lithium-ion diffusion kinetics in the ternary system. This study establishes a high-performance low-temperature 18650 battery chemistry and provides quantitative mechanistic insights into how dimensional synergy in conductive additive design governs the rate capability, thermal behavior, and cycling stability of nickel-rich cathodes operating under extreme conditions.

