Size-dependent activity of carbon dots for photocatalytic H2 generation in combination with a molecular Ni cocatalyst

Casadevall, Carla, Lage, Ava, Mu, Manting, Greer, Heather F., Antón-García, Daniel, Butt, Julea N. ORCID: https://orcid.org/0000-0002-9624-5226, Jeuken, Lars J. C., Watson, Graeme W., Garcia-Melchor, Max and Reisner, Erwin (2023) Size-dependent activity of carbon dots for photocatalytic H2 generation in combination with a molecular Ni cocatalyst. Nanoscale, 15 (38). pp. 15775-15784. ISSN 2040-3364

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Abstract

Carbon dots (CDs) are low-cost light-absorbers in photocatalytic multicomponent systems, but their wide size distribution has hampered rational design and the identification of the factors that lead to their best performance. To address this challenge, we report herein the use of gel filtration size exclusion chromatography to separate amorphous, graphitic, and graphitic N-doped CDs depending on their lateral size to study the effect of their size on photocatalytic H 2 evolution with a DuBois-type Ni cocatalyst. Transmission electron microscopy and dynamic light scattering confirm the size-dependent separation of the CDs, whereas UV-vis and fluorescence spectroscopy of the more monodisperse fractions show a distinct response which computational modelling attributes to a complex interplay between CD size and optical properties. A size-dependent effect on the photocatalytic H 2 evolution performance of the CDs in combination with a molecular Ni cocatalyst is demonstrated with a maximum activity at approximately 2-3 nm CD diameter. Overall, size separation leads to a two-fold increase in the specific photocatalytic activity for H 2 evolution using the monodisperse CDs compared to the as synthesized polydisperse samples, highlighting the size-dependent effect on photocatalytic performance.

Item Type: Article
Additional Information: Funding information: Financial support from the BBSRC (BB/S00159X/1, BB/S002499/1 and BB/S000704/1), the European Commission for Horizon 2020 Marie Skłodowska-Curie Individual Fellowships (890745-SmArtC, C. C), and the Science Foundation Ireland (SFI20/FFP-P/8740, M. G.-M.). The EPSRC Multi-User Equipment Call (EP/P030467/1) is also thanked.
Uncontrolled Keywords: materials science(all),3* ,/dk/atira/pure/subjectarea/asjc/2500
Faculty \ School: Faculty of Science > School of Chemistry
Faculty of Science > School of Biological Sciences
UEA Research Groups: Faculty of Science > Research Groups > Centre for Photonics and Quantum Science
Faculty of Science > Research Groups > Molecular Microbiology
Faculty of Science > Research Groups > Energy Materials Laboratory
Faculty of Science > Research Groups > Chemistry of Light and Energy
Faculty of Science > Research Groups > Chemistry of Life Processes
Faculty of Science > Research Centres > Centre for Molecular and Structural Biochemistry
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Depositing User: LivePure Connector
Date Deposited: 01 Sep 2023 08:30
Last Modified: 13 Oct 2023 00:43
URI: https://ueaeprints.uea.ac.uk/id/eprint/92961
DOI: 10.1039/D3NR03300G

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