Carbon Dots Enabling Parts-Per-Billion Sensitive and Ultraselective Photoluminescence Lifetime-Based Sensing of Inorganic Mercury

One of the UN Sustainable Development Goals is to ensure universal access to clean drinking water. Among the various types of water contaminants, mercury (Hg) is considered to be one of the most dangerous ones. It is mostly its immense toxicity and vast environmental impact that stand out. To tackle...

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Detalles Bibliográficos
Autores: Zdražil, Lukáš, Panáček, David, Sedajová, Veronika, Baďura, Zdeněk, Langer, Michal, Medveď, Miroslav, Paloncýová, Markéta, Scheibe, Magdalena, Kalytchuk, Sergii, Zoppellaro, Giorgio, Kment, Štěpán, Cadranel, Alejandro, Bakandritsos, Aristides, Guldi, Dirk, Otyepka, Michal, Zbořil, Radek
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:Argentina
Institución:Consejo Nacional de Investigaciones Científicas y Técnicas
Repositorio:CONICET Digital (CONICET)
Idioma:inglés
OAI Identifier:oai:ri.conicet.gov.ar:11336/228653
Acceso en línea:http://hdl.handle.net/11336/228653
Access Level:acceso abierto
Palabra clave:CARBON DOTS
COLLOIDAL NANOMATERIALS
MERCURY SENSING
TIME-RESOLVED PHOTOLUMINESCENCE
https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
Descripción
Sumario:One of the UN Sustainable Development Goals is to ensure universal access to clean drinking water. Among the various types of water contaminants, mercury (Hg) is considered to be one of the most dangerous ones. It is mostly its immense toxicity and vast environmental impact that stand out. To tackle the issue of monitoring water quality, a nanosensor based on carbon dots (CDs) is developed, whose surface is functionalized with carboxylic groups. CDs show Hg2+ concentration-dependent photoluminescence (PL) lifetimes along with an ultrahigh sensitivity and selectivity. The selectivity of PL quenching by Hg2+ is rationalized by performing light-induced electron paramagnetic resonance (LEPR) spectroscopy showing significant perturbation of the CD photoexcited state upon Hg2+ binding. The experimental findings are supported by time-dependent density functional theory (TD-DFT) calculations. These unveiled the emergence of a low-lying charge transfer state involving a vacant 6s orbital of Hg2+ stabilized by relativistic effects.