28 May Single-step construction of architected hybrid interphases: A robust strategy for high energy density batteries Back to Sci. Publications

ABSTRACT

Ni-rich layered oxides are promising cathode materials for lithium-based batteries due to their high energy density. However, their long-term performance is limited by interfacial and structural instabilities during cycling. To address this, we developed an intertwined hybrid network that forms a robust artificial cathode–electrolyte interphase (CEI) via a simple one-step wet impregnation process without thermal treatment. The hybrid network combines a lithium single ion conducting polymer (SICP) for ionic transport, multi-walled carbon nanotubes (MWCNTs) for electronic conductivity, and polyvinylpyrrolidone (PVP) to ensure uniform dispersion. This synergistic architecture enhances coupled ionic–electronic transport and improves interfacial kinetics, leading to greater electrochemical stability. As a result, coated Ni-rich cathodes show significantly improved cycling performance in both liquid and solid-state systems under pressure-free conditions. In liquid electrolytes, the coated material retains 64% capacity after 200 cycles, compared to 41% after 100 cycles for the pristine material. In solid-state cells, it retains 55% capacity after 45 cycles, outperforming the pristine material (59% after 20 cycles). This scalable approach provides an effective strategy for stabilizing high-energy cathodes and is applicable to various battery architectures.

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