Electrolyte-Impregnated Mesoporous Hollow Microreactor to Supplement an Inner Reaction Pathway for Boosting the Cyclability of Li-CO2Batteries

Li-CO2batteries that integrate energy storage with greenhouse gas fixation have received a great deal of attention in the pursuit of carbon neutrality. However, cyclic accumulation of the insulative and insoluble Li2CO3on the cathode surface severely restrains the battery cyclability, especially under a high depth of discharge/charge. Herein, we design and fabricate a microreactor-type catalyst by embedding Ru nanoparticles into the shells of mesoporous hollow carbon spheres. We show that both the hollow cavity and mesoporous shell are indispensable for concertedly furnishing a high activity to catalyze reversible Li2CO3formation/decomposition. This unique structure ensures that the Ru sites masked by exterior Li2CO3deposits during charging can resume the redox process of discharge by working with the prestored electrolyte to establish an inner reaction path. The thus fabricated Li-CO2batteries demonstrate remarkable cyclability of 1085 cycles under 0.5 Ah g–1and 326 cycles under 2 Ah g–1at 1 A g–1, outshining most of the literature reports. This study highlights a smart catalyst design to boost the reversibility and cyclability of Li-CO2batteries through an “in & out” strategy.