Double spatial confinement on ruthenium nanoparticles inside carbon frameworks as durable catalysts for a quasi‐solid‐state Li–O₂ battery

Abstract The rational design of large‐area exposure, nonagglomeration, and long‐range dispersion of metal nanoparticles (NPs) in the catalysts is critical for the development of energy storage and conversion systems. Little attention has been focused on modulating and developing catalyst interface contact engineering between a carbon substrate and dispersed metal. Here, a highly dispersed ultrafine ruthenium (Ru) NP strategy by double spatial confinement is proposed, that is, incorporating directed growth of metal–organic framework crystals into a bacterial cellulose templating substrate to integrate their respective merits as an excellent electrocatalytic cathode catalyst for a quasi‐solid‐state Li–O₂ battery. The porous carbon matrix with highly dispersed ultrafine Ru NPs is well designed and used as cathode catalysts in a Li–O₂ battery, demonstrating a high discharge areal capacity of 6.82 mAh cm^–2 at 0.02 mA cm^–2, a high‐rate capability of 4.93 mAh cm^–2 at 0.2 mA cm^–2, and stable discharge/charge cycling for up to 500 cycles (2000 h) with low overpotentials of ~1.4 V. This fundamental understanding of the structure–performance relationship demonstrates a new and promising approach to optimize highly efficient cathode catalysts for solid‐state Li–O₂ batteries.