Title: Magnetic Polaron States in Photoluminescent Carbon Dots Enable Hydrogen Peroxide Photoproduction

Authors: Lukáš Zdražil, Zdenek Baďura, Michal Langer, Sergii Kalytchuk, David Panáček, Magdalena Scheibe, Štepán Kment, Hana Kmentová, Muhammed Arshad Thottappali, Elmira Mohammadi, Miroslav Medveď, Aristides Bakandritsos, Giorgio Zoppellaro, Radek Zbořil and Michal Otyepka

DOI: https://doi.org/10.1002/smll.202206587

Abstract: Photoactivation of aspartic acid-based carbon dots (Asp-CDs) induces the generation of spin-separated species, including electron/hole (e−/h+) polarons
and spin-coupled triplet states, as uniquely confirmed by the light-induced electron paramagnetic resonance spectroscopy. The relative population of
the e−/h+ pairs and triplet species depends on the solvent polarity, featuring a substantial stabilization of the triplet state in a non-polar environment
(benzene). The electronic properties of the photoexcited Asp-CDs emerge from their spatial organization being interpreted as multi-layer assemblies
containing a hydrophobic carbonaceous core and a hydrophilic oxygen and nitrogen functionalized surface. The system properties are dissected theoretically
by density functional theory in combination with molecular dynamics simulations on quasi-spherical assemblies of size-variant flakelike model systems,
revealing the importance of size dependence and interlayer effects. The formation of the spin-separated states in Asp-CDs enables the photoproduction
of hydrogen peroxide (H2O2) from water and water/2-propanol mixture via a water oxidation reaction.