Abstract
AbstractImproving the round‐trip efficiency and cycle life of lithium‐oxygen batteries (LOBs) through the cathode design is essential for their employment in electric vehicles. Here, a neoteric chimeric air‐cathode is proposed, in which ultra‐dispersed ruthenium (Ru) nanoparticles are partially confined by microtube walls of free‐standing carbon textiles, but petty parts of Ru with catalytic surfaces are exposed. The special chimeric structure benefits not only for preventing nanocatalysts agglomeration but also tailoring the formation/decomposition mechanisms of lithium peroxide (Li2O2) during oxygen reduction/evolution reactions. Critically, theoretical simulations disclose that the enlarged chimeric catalyst‐support interphase between the Ru and carbon matrix enhances the electron density of Ru particles and then induces a gradient Gibbs free energy of LiO2 adsorption energy at active sites, and thus fundamentally modulates the morphology evolution mechanism of finial Li2O2. In the LOBs, the chimeric electrode affords a remarkably high energy efficiency of 84.1% and long‐term cyclability (260 cycles at 300 mA g−1).
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