Solid–Polymer–Electrolyte Interphase Inductively Formed by Surface Chemistry to Stabilize the High Ni Cathode in Sulfide-Based All-Solid-State Lithium Batteries

Abstract

High-nickel cathode, LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811), and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries (ASSLBs). However, this combination faces the issue of interfacial instability between the cathode and electrolyte. Given the surface alkalinity of NCM811, we propose a strategy to construct a solid–polymer–electrolyte (SPE) interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules. As a proof-of-concept, this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous, compact, and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li₆PS₅Cl solid-state electrolyte. Consequently, the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^–1 at 0.2 C, 160.9 mA h g^–1 at 2.0 C and 112.3 mA h g^–1 at 10 C, and particularly, excellent long-term cycling stabilities over 11000 cycles with a 71.95% capacity retention at 10 C at 25°C, as well as a remained capacity of 117.9 mA h g^–1 after 8000 cycles at 30 C at 60°C, showing a great application prospect. This study provides a new route for creating electrochemically and structurally stable solid–solid interfaces for ASSLBs.

Keywords

all-solid-state lithium batteries / Ni-rich layered oxides / nucleophilic reaction / solid–polymer–electrolyte interphase / sulfide solid electrolyte

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