Person:

Sedenho, Graziela Cristina

Microbatteries with safe, non-corrosive electrolyte chemistries can have an immediate positive impact on modern life applications, such as ingestible electronic pills and system-on-chip bioelectronics. Here a safe, non-corrosive and non-flammable microbattery is reported. A natural agarose hydrogel is the electrolyte-supporting matrix, and organic and organometallic molecules are the redox-active species. This device can safely meet the needs of ingestible medical microdevices as a primary battery. Additionally, this redox gel system can be used as a secondary battery for on-chip electronics applications, potentially enabling safe and cost-effective small-scale energy storage.

Quinones can undergo thermodynamically reversible proton-coupled electron transfer reactions and are being applied as electroactive compounds in aqueous organic batteries. However, the electrochemical reversibility of these compounds is affected not only by their molecular structure but also by the properties of a carbon-based electrode surface. This study combines experimental and theoretical approaches to understand this dependence. We study the electron transfer kinetics of two synthesized quinone derivatives and two commercially available ones with a glassy carbon, a highly ordered pyrolytic graphite, and a high-edge-density graphite electrode (HEDGE). The electrochemical reversibility is notably improved on the HEDGE, which shows a higher density of defects and presents oxygenated functional groups at its surface. The electron transfer kinetics are controlled by adsorbed species onto the HEDGE. Molecular dynamics simulation and quantum mechanics calculations suggest defects with oxygen-containing functional groups, such as C–O and C═O, on HEDGE surfaces drive the interaction with the functional groups of the molecules, during physisorption from van der Waals forces. The presence of sulfonic acid side groups and a greater number of aromatic rings in the molecular structure may contribute to a higher stabilization of quinone derivatives on HEDGEs. We propose that high-performance carbon-based electrodes can be obtained without catalysts for organic batteries, by the engineering of carbon-based surfaces with edge-like defects and oxygenated functional groups.