Defect-Driven Ionic Trap Construction and Interface Modulation for Rapid Li+ Kinetics in Composite Solid Electrolytes

Jiaming Wen

doi:10.1002/adma.202519541

Defect-Driven Ionic Trap Construction and Interface Modulation for Rapid Li+ Kinetics in Composite Solid Electrolytes

2025-12-01

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DOI：10.1002/adma.202519541

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Composite solid electrolytes (CSEs) hold great promise for lithium metal batteries owing to the inherent safety and mechanical flexibility, yet their progress is impeded by sluggish Li+ transport and unstable interfacial chemistry. Herein, we unveil an ionic-trap framework to clarify the essential role of inorganic fillers in regulating ion migration. Specifically, milled carbon nitride with oxamide incorporation (MCNOI) introduces abundant nitrogen vacancies that function as a shallow ionic trap, enabling reversible Li+ capture/release and constructing continuous conduction pathways. By contrast, traditional carbon nitride forms a deep ionic trap that immobilizes Li+, whereas ionic trap-free polymer electrolytes lack effective guidance for Li+ transport. Beyond intrinsic ion conduction, MCNOI facilitates the formation of a gradient organic-inorganic interphase, redistributing interfacial charges, suppressing anion migration, and promoting uniform Li deposition. Consequently, the optimized CSE achieves a high Li+ transference number (0.68), ultralong cycling stability (>3000 h), and remarkable full-cell durability (92.3% capacity retention after 1800 cycles at 5 C). These findings highlight defect-engineered fillers as active regulators of Li+ transport, redefining design strategies for durable high-performance solid-state batteries.

Keywords:

carbon nitride

composite solid electrolyte

interface modulation

shallow ionic trap

Defect-Driven Ionic Trap Construction and Interface Modulation for Rapid Li+ Kinetics in Composite Solid Electrolytes

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