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http://hdl.handle.net/1942/33191
Title: | Photogenerated charge collection on diamond electrodes with covalently linked chromophore monolayers | Authors: | RAYMAKERS, Jorne Artemenko, A VERSTRAETEN, Frederik Krysova, H Cermak, J NICLEY, Shannon Lopez-Carballeira, D Kromka, A HAENEN, Ken Kavan, L MAES, Wouter Rezek, B |
Issue Date: | 2020 | Publisher: | PERGAMON-ELSEVIER SCIENCE LTD | Source: | ELECTROCHIMICA ACTA, 337 (Art N° 135762) | Abstract: | Encouraged by its rich surface chemistry and excellent electrochemical properties, boron-doped nanocrystalline diamond (B:NCD) is a promising p-type photoelectrode in dye-sensitized solar cells. One method of diamond surface functionalization using stable carbon-carbon bonds involves the electrochemical grafting of diazonium salts. However, this method typically leads to multilayers that may complicate the transport of photogenerated charges. Here, we establish functionalization of B:NCD electrodes by a monolayer of ethynylphenyl molecules using sterically hindered 4-(trimethylsilyl)ethynylbenzenediazonium tetrafluoroborate. Both the density and structural orientation of the grafted layer are investigated by angular resolved X-ray photoelectron spectroscopy, confirming the presence of covalently grafted monolayers. After removal of the trimethylsilyl protective groups, the resulting ethynyl functionalities are employed to immobilize organic donor-acceptor chromophores via Sonogashira cross-coupling reactions. Homogenous surface coverage is achieved even on the B:NCD electrode. Atomic scale DFT computing reveals that for the chromophore with the strongest acceptor unit, efficient charge separation of 20 angstrom is obtained where photogenerated holes move directly into diamond. Yet, photocurrent and photovoltage measurements suggest competitive electron recombination to the diamond electrode via the redox electrolyte. Correlation between the density of the molecular layer and photocurrents/photovoltage provides better understanding of the charge generation and recombination pathways in diamond-organic photoelectrochemical cells. (C) 2020 Elsevier Ltd. All rights reserved. | Keywords: | Boron-doped diamond;Surface functionalization;Sonogashira cross-coupling;Monolayers;Photoelectrochemistry | Document URI: | http://hdl.handle.net/1942/33191 | ISSN: | 0013-4686 | e-ISSN: | 1873-3859 | DOI: | 10.1016/j.electacta.2020.135762 | ISI #: | WOS:000521531700059 | Rights: | 2020 Elsevier Ltd. All rights reserved | Category: | A1 | Type: | Journal Contribution | Validations: | ecoom 2021 |
Appears in Collections: | Research publications |
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File | Description | Size | Format | |
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Manuscript - Raymakers et al.pdf | Peer-reviewed author version | 1.33 MB | Adobe PDF | View/Open |
1-s2.0-S0013468620301547-main.pdf Restricted Access | Published version | 1.7 MB | Adobe PDF | View/Open Request a copy |
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