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Site-specific self-protection of stacking faults enables durable Li-gas batteries
Yuchun Liu1, Tianqi Liu1, Xinyun Wang1
1Hefei National Research Center for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China.
Abstract:
Rechargeable Li-gas batteries, represented by Li-O2 and Li-CO2 systems, are promising for high-energy-density storage and gas-involved energy conversion, yet their operation is constrained by the trade-off between catalytic activity and structural durability of cathodes. Metastable defects such as stacking faults offer active sites for accelerating sluggish gas redox reactions, but readily undergo electrochemical stress-induced slip and structural collapse during cycling. Inspired by plant traumatic resinosis, we propose a site-specific self-protection strategy that exploits the intrinsic anisotropy of stacking faults to decouple catalytic reaction planes from orthogonal protective functional planes. On the reaction plane, over-coordinated dislocation sites amplify surface electrostatic potential differences and promote Li2CO3 decomposition via nucleophilic/electrophilic interactions. On the functional plane, selective interactions with sulfur-containing electrolyte components induce in situ reconstruction of a multiphase inorganic-organic amorphous interphase, anchoring stacking faults without blocking catalytic sites. As a Li-CO2 proof of concept, stacking-fault-rich molybdenum boride (MoB) delivers 90.13% average energy efficiency over 2500 h and stable operation at 150 °C for nearly 500 h. This work establishes a self-protection paradigm for stable metastable active structures and provides a universal interface design principle for durable Li-gas batteries.