Computational design of donor-acceptor stacked polycyclic aromatic hydrocarbons as photocatalytic sites in carbon dots
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Dátum
2025
Názov časopisu
ISSN časopisu
Názov zväzku
Vydavateľ
The Royal Society of Chemistry : Cambridge
ISBN
ISSN
2040-3364
2040-3372
2040-3372
Abstrakt
Carbon dots (CDs) are complex carbon-based nanomaterials with exceptional photoluminescence characteristics and great promise for sustainable metal-free photocatalysis. However, their structural heterogeneity poses a major challenge for the rational design and prediction of photocatalytic performance. To overcome this limitation, we propose a bottom-up strategy centered on CD-inspired systems with well-defined molecular architecture. Specifically, we computationally screened 5700 stacked polycyclic aromatic hydrocarbon aggregates, as representatives of CD aromatic domains, to identify donor–acceptor pairs capable of efficient charge separation under photoexcitation. Using a few carefully chosen molecular descriptors and a computationally efficient protocol, we identified best candidate systems for oxidative and reductive quenching pathways. Subsequent time-dependent density functional theory analysis confirmed that these systems exhibit key photocatalytic features: a charge-transfer character in the lowest excited state, well-separated bright local excitations, favorable redox potentials, and propensity for extended aggregation with core-surface charge separation. Our approach not only offers a practical design route for CD-like photocatalysts but also provides the fundamental understanding needed to engineer tunable, efficient, and sustainable donor–acceptor photocatalytic systems.
Popis
In: Nanoscale. Cambridge : The Royal Society of Chemistry, 2025. ISSN 2040-3364. Vol. 17, no. 39 (2025), pp. 22834-22848.
Kľúčové slová
aromatizácia, aromatization, uhlík, carbon, prenos náboja, návrhy, polycyklické aromatické uhľovodíky, polyaromatické uhľovodíky, polycylic aromatic hydrocarbons, polyaromatic hydrocarbons, PAH, uhlíkové bodky, carbon dots, fotokatalytické miesta, photocatalytic sites, teória funkcionálu hustoty, redoxné reakcie
Výstup z projektu
Moravian-Silesian Region 00734/2023/RRC Experimental and theoretical studies of near-infrared-emitting and chiral carbon dot luminophores project
TAČR CZ.02.01.01/00/22_008/0004587 TECHSCALE: Technologie za hranicí nanosvěta
APVV-20-0098 Svetlom riadené molekulové prepínanie
COST CA21101 COST Action - Confined molecular systems: from a new generation of materials to the stars (cosy)
APVV-21-0346 Modifikácia povrchov ako bariéra pre adsorpciu proteínov
VEGA 2/0098/23 In situ redukcia grafén oxidu asistovaná polymérnymi reťazcami: výpočtová a experimentálna štúdia
Ministerstvo školstva, mládeže a telovýchovy ČR 90254 e-INFRA CZ
Ina CZ.10.03.01/00/22_003/0000048 REFRESH - Research Excellence For Region Sustainability and High-tech Industries
Citácia
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CC BY Creative Commons Attribution 4.0. International
info:eu-repo/semantics/openAccess
info:eu-repo/semantics/openAccess