Anionic Vacancy-dependent Activity of CoSe2 with Tunable Interfacial Electronic Structure on N-doped Carbon Cloth Endowing Advanced Li-O2 Battery

The inferior reversibility of the formation/decomposition of lithium peroxide (Li2O2) with the insolubility and insulation features results in poor energy efficiency and limited durability of the state-of-the-art Li-O2 batteries. Herein, we elaborately design the sisal-like CoSe2 nanowires enriched with Se vacancies (VSe-CoSe2) anchoring on the scaffold of magnetron sputtered N-doped carbon cloth (N-CC) to address the above challenges. The synergistic coupling of vacancy regulation with interfacial interaction can tune the ability to adsorb active oxygen and intermediate species and boost the interfacial electron transfer during oxygen redox reactions. Experimental result demonstrates that the VSe-CoSe2@N-CC based Li-O2 battery demonstrates substantially decreased overpotential (~ 0.56 V) and extraordinarily durability (over 955 h). This work indicates that the synergistic coupling of vacancy modulation and interface interaction is a promising strategy for effectively enhancing the comprehensive performance of Li-O2 batteries, which provides prospective insights into the exploration of next-generation highly efficient metal-air batteries.