Abstract
Cross-linking poly(glycidyl methacrylate) microparticles with redox-responsive bis(5-amino-l,3,4-thiadiazol-2-yl) disulfide moieties yield redox-active particles (RAPs) capable of electrochemical energy storage via a reversible 2-electron reduction of the disulfide bond. The resulting RAPs show improved electrochemical reversibility compared to a small-molecule disulfide analogue in solution, attributed to spatial confinement of the polymer-grafted disulfides in the particle. Galvanostatic cycling was used to investigate the impact of electrolyte selection on stability and specific capacity. A dimethyl sulfoxide/magnesium triflate electrolyte was ultimately selected for its favorable electrochemical reversibility and specific capacity. Additionally, the specific capacity showed a strong dependence on particle size where smaller particles yielded higher specific capacity. Overall, these experiments offer a promising direction in designing synthetically facile and electrochemically stable materials for organosulfur-based multielectron energy storage coupled with beyond Li ion systems such as Mg.
Highlights
Cross-linking poly(glycidyl methacrylate) microparticles with redox-responsive bis(5-amino-l,3,4-thiadiazol-2-yl) disulfide moieties yield redox-active particles (RAPs) capable of electrochemical energy storage via a reversible 2-electron reduction of the disulfide bond
The ability to systematically tune the structure of organic materials allows fine-tuning of their electrochemical behavior/stability, and the raw materials for organic systems are generally more abundant compared to many of the key metal oxides employed in inorganic systems, offering an advantage when considering renewable/sustainable technologies
ACS Macro Letters pubs.acs.org/macroletters substrate. This technique is utilized in current Li+-ion battery metal oxide electrodes and has been demonstrated with organic materials; for example, suspensions of polyaniline particles have been shown to charge more thoroughly than polyaniline films.[14]
Summary
Cross-linking poly(glycidyl methacrylate) microparticles with redox-responsive bis(5-amino-l,3,4-thiadiazol-2-yl) disulfide moieties yield redox-active particles (RAPs) capable of electrochemical energy storage via a reversible 2-electron reduction of the disulfide bond. Results showed that no additional 1-SS-1 was detected in the solution during a second UV annealing process, consistent with the removal of x-SS-1 from P2 and the formation of the more densely cross-linked P2-SS containing only disulfide cross-linkers x-SS-x.
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