Magnetic Polaron States in Photoluminescent Carbon Dots Enable Hydrogen Peroxide Photoproduction
Status PubMed-not-MEDLINE Jazyk angličtina Země Německo Médium print-electronic
Typ dokumentu časopisecké články
Grantová podpora
CZ.1.05/2.1.00/19.0377
Ministry of Education, Youth and Sports of the Czech Republic
Ministry of Education, Youth and Sports of the Czech Republic
02.1.01/0.0/0.0/15_003/0000416
Operational Program Research, Development and Education
02.1.01/0.0/0.0/16_019/0000754
Operational Program Research, Development and Education
APVV-20-0098
Slovak Research and Development Agency
22-02005S
Grantová Agentura České Republiky
CA21101
European Cooperation in Science and Technology
IGA_PrF_2022_019
Univerzita Palackého v Olomouci
ID:90140
Ministerstvo Školství, Mládeže a Tělovýchovy
22-26416S
Czech Science Foundation
22-02005S
Czech Science Foundation
PubMed
37038085
DOI
10.1002/smll.202206587
Knihovny.cz E-zdroje
- Klíčová slova
- carbon dots, density functional theory, high spin species, hydrogen peroxide, photoluminescence, polarons, water oxidation,
- Publikační typ
- časopisecké články MeSH
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 (H2 O2 ) from water and water/2-propanol mixture via a water oxidation reaction.
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