Abstract
To develop a lithium–oxygen (Li–O2) battery with a high specific energy, the electrochemical oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have been systematically investigated on gold and porous carbon electrodes in a DMSO-based electrolyte solution containing tetrathiafulvalene (TTF) as a redox mediator by using in situ UV–vis absorption spectroscopy and surface-enhanced Raman vibrational spectroscopy (SERS) in combination with ex situ infrared and Raman spectroscopies. Our results demonstrate that TTF definitely reduces the overpotential for the OER process and restrains the decomposition of the carbon electrode and solvent during the OER, while the functionality of the redox mediator can change with the electrode materials and morphologies. No free TTF+ was observed in solution during a round-trip galvanostatic ORR/OER cycle on the gold electrode surface. The electrochemically generated TTF+ was mainly consumed by the oxidative decomposition of lithium superoxide (LiO2) in soluti...
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