Non-equilibrium thermodynamics in electrochemical complexation of Li–oxygen porous electrodes

Abstract

The lithium–oxygen conversion chemistry relies on solid-electrolyte interface centered energy storage, rather than bulk considerations in intercalation chemistry. The electrochemical complexations in porous air electrodes are, however, a manifestation of coupled interface-transport-kinetic interactions. The non-equilibrium thermodynamics behind such multi-modal coupling, hitherto unappreciated, forms the central argument of this work. We comprehensively demonstrate the role of reciprocity between electrode architecture and off-equilibrium interactions in Li–O₂ electrochemistry based energy storage.