Nanoparticle-Polymer Surface Functionalizations for Capacitive Energy Storage: Experimental Comparison to First Principles Simulations

Dielectric capacitors present many advantages for large-scale energy storage, but they presently require higher energy density. We demonstrate novel high energy density polymer-nanoparticle composite capacitors utilizing thiol-ene click chemistry surface groups to bond the nanoparticles covalently to the polymer matrix. Interfacial effects in composites cannot be observed directly, and in our previous work, we examined the nanoparticle-polymer interface in silico. In this work, we experimentally examine the five surface functionalizations modeled previously, fabricating high energy density thin film capacitors to test our predictions. Results from this study, in conjunction with properties previously determined in silico, further improve the understanding of the role of surface functionalizations in composites prepared using click chemistry. The coating density of the surface functionalizations is shown to be a key factor in relating our computational results to experimental results. We show how using both coating density and our previous modeling in combination allows for prescreening of surface functionalizations for future composites, reducing experimental cost. We also demonstrate high energy density capacitors with ~20 J/cm³.