title: Mechanistic Insights into the Challenges of Cycling a Nonaqueous Na-O2Battery.
abstract: Superoxide-based nonaqueous metal-oxygen batteries have received considerable research attention as they exhibit high energy densities and round-trip efficiencies. The cycling performance, however, is still poor. Here we study the cycling characteristic of a Na-O2battery using solid-state nuclear magnetic resonance, Raman spectroscopy, and scanning electron microscopy. We find that the poor cycling performance is primarily caused by the considerable side reactions stemming from the chemical aggressiveness of NaO2as both a solid-phase and dissolved species in the electrolyte. The side reaction products cover electrode surfaces and hinder electron transfer across the electrode-electrolyte interface, being a major reason for cell failure. In addition, the available electrode surface and porosity change considerably during cell discharging and charging, affecting the diffusion of soluble species (superoxide and water) and resulting in inhomogeneous reactions across the electrode. This study provides insights into the challenges associated with achieving long-lived superoxide-based metal-O2batteries.
authors.affiliation: Chemistry Department, University of Cambridge , Lensfield Road, Cambridge, United Kingdom CB2 1EW.
authors.forename: Tao
authors.initials: T
authors.lastname: Liu
authors.affiliation: Chemistry Department, University of Cambridge , Lensfield Road, Cambridge, United Kingdom CB2 1EW.|Cambridge Graphene Centre, University of Cambridge , Cambridge, United Kingdom CB3 0FA.
authors.forename: Gunwoo
authors.initials: G
authors.lastname: Kim
authors.affiliation: Chemistry Department, University of Cambridge , Lensfield Road, Cambridge, United Kingdom CB2 1EW.
authors.forename: Mike T L
authors.initials: MT
authors.lastname: Casford
authors.affiliation: Chemistry Department, University of Cambridge , Lensfield Road, Cambridge, United Kingdom CB2 1EW.
authors.forename: Clare P
authors.initials: CP
authors.lastname: Grey