Engineering Li+ Transport in Ni-Rich Layered Cathodes Toward Homogenization
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Published on: November 11, 2013
Lili Lin1, Min Du1, Jiatao Lou1
1Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, China.
Abstract:
Nickel-rich layered oxide (NRLO) cathodes (Ni≥80%) are promising for next-generation lithium-ion batteries with energy densities exceeding 300 Wh kg-1, but suffer from rapid degradation under deep delithiation, including phase transitions, microcracking, and surface reconstruction. These failure modes are increasingly recognized to be coupled through heterogeneous Li+ transport across multiple length scales. Here we show that spatial variations in Li+ transport originate from atomic, structural, and interfacial factors and ultimately evolve into macroscopic chemo-mechanical degradation. On this basis, we introduce transport homogenization as a unifying design principle for regulating Li+ transport in NRLO cathodes. Within this framework, diverse material engineering strategies, including bulk structural design, interfacial transport engineering, and dynamic transport regulation, are interpreted from a common transport-centered perspective. We further summarize emerging characterization approaches for quantifying transport heterogeneity and discuss future opportunities for establishing predictive cross-scale design principles. Overall, this review establishes a transport-centered framework that unifies degradation in NRLO cathodes and provides a mechanistic basis for rational design of next-generation high-energy-density cathode materials.
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