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Particle Crust Engineering of Cathode Materials for High-Performance Lithium-Ion Batteries
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DOI：10.1021/accountsmr.6c00020.png)
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Abstract
En 中文
ConspectusThe rapid expansion of the green electric vehicle market has spurred the development of next-generation lithium-ion batteries (LIBs) with energy densities approaching 500 Wh/kg and beyond. Achieving these ambitious energy targets requires the advancement of high-capacity cathode materials such as nickel-rich layered oxides. However, the practical deployment of these cathodes is often hindered by insufficient stability and reliability, primarily due to accelerated degradation at the cathode–electrolyte interface. Under high-voltage conditions, which are critical for maximizing specific capacity, these interfaces become hotspots for parasitic reactions, including transition metal dissolution, electrolyte decomposition, oxygen release, and phase transformations. Such reactions not only lead to rapid capacity fading but also raise significant safety concerns. Consequently, enhancing the stability of the cathode–electrolyte interface has emerged as a crucial challenge, attracting considerable attention from both academic researchers and industry stakeholders.Constructing protective coating layers on cathode particles is one of the most straightforward strategies for stabilizing the cathode–electrolyte interface, yet these artificially engineered coatings often introduce new challenges, such as impaired interfacial charge transport and the risk of delamination during cycling. These limitations highlight the necessity of fundamentally tailoring the surface chemistry of cathode materials to design more ideal and intrinsically stable interfaces for next-generation LIBs, which require advanced interfacial control to create well-defined model systems that can serve as reliable platforms for performance evaluation and mechanistic studies. However, reliable methods for constructing uniform and conformal coatings with nanometer precision are currently limited. While dry coating processes are commonly employed in industry, achieving a homogeneous and continuous ultrathin film over complex cathode particle morphologies remains challenging. Chemical vapor deposition techniques can produce high-quality nanofilms, yet their practical adoption is often hindered by a limited range of achievable coating materials and concerns regarding economic viability, including low throughput and technical complexity. In contrast, wet-chemistry methods provide a promising alternative, enabling the cost-effective and scalable fabrication of a diverse array of conformal nanoscale layers.This Account summarizes our systematic efforts to advance particle crust engineering as a transformative strategy for stabilizing high-energy cathode materials. Here, “particle crust engineering” is defined as the precise design of the cathode surface into an integrated shell. We begin by detailing wet-chemical synthesis strategies that facilitate the formation of uniform coatings with nanometer-scale precision. By carefully controlling precipitation kinetics through methods including gradual release of precipitants, coordination modulation, and catalyst assistance, we have successfully achieved robust deposition of metal oxides, phosphates, sulfides, and carbon layers, establishing ideal core–shell model systems for interfacial studies. Moving beyond conventional inert shells, we demonstrate how these tailored coatings can serve as reactants and be transformed via heat treatment into multifunctional “crust”, including Li+ conductors, doped crusts, and hybrid surface architectures, thereby effectively decoupling the traditional trade-off between interfacial stability and charge transfer kinetics. This approach has been successfully applied in both liquid-electrolyte LIBs and all-solid-state batteries. Looking ahead, we identify several key frontiers for the field and anticipate that this Account will inspire new endeavors in the development of advanced particle crusts for cathode materials, ultimately contributing to the advancement of high-performance lithium batteries.
Keywords:
particle crust engineering
cathode materials
lithium-ion batteries
interfacial stability
nanoscale coatings
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