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Cobaloxime complex salts : synthesis, patterning on carbon nanomembranes and heterogeneous hydrogen evolution studies
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Oswald, Eva, Gaus, Anna-Laurine, Kund, Julian, Küllmer, Maria, Romer, Jan, Weizenegger, Simon, Ullrich, Tobias, Mengele, Alexander K., Petermann, Lydia, Leiter, Robert, Unwin, Patrick R., Kaiser, Ute, Rau, Sven, Kahnt, Axel, Turchanin, Andrey, von Delius, Max and Kranz, Christine (2021) Cobaloxime complex salts : synthesis, patterning on carbon nanomembranes and heterogeneous hydrogen evolution studies. Chemistry – A European Journal, 27 (68). pp. 16896-16903. doi:10.1002/chem.202102778 ISSN 1521-3765.
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Official URL: https://doi.org/10.1002/chem.202102778
Abstract
Cobaloximes are promising, earth-abundant catalysts for the light-driven hydrogen evolution reaction. Typically, these cobalt(III) complexes are prepared in situ or employed in their neutral form, e.g. [Co(dmgH 2 )(py)Cl], even though related complex salts have been reported previously and could in principle offer improved catalytic activity as well as more efficient immobilization on solid support. Here we report an interdisciplinary investigation into complex salts [Co(dmgH) 2 (py) 2 ] + [Co(dmgBPh 2 ) 2 Cl 2 ] - , TBA + [Co(dmgBPh 2 ) 2 Cl 2 ] - and [Co(dmgH) 2 (py) 2 ] + BArF - . We describe their strategic syntheses from commercially available complex [Co(dmgH) 2 (py)Cl] and demonstrate that these double and single complex salts are potent catalysts for the light-driven hydrogen evolution reaction. We also show that scanning electrochemical cell microscopy can be used to deposit arrays of catalysts [Co(dmgH) 2 (py) 2 ] + [Co(dmgBPh 2 ) 2 Cl 2 ] - and [Co(dmgH) 2 (py)Cl] on supported and free-standing amino-terminated ~ 1 nm thick carbon nanomembranes (CNMs). Photocatalytic H 2 evolution at such arrays was quantified with Pd microsensors using scanning electrochemical microscopy, thus providing a new approach for catalytic evaluation and opening up novel routes for the creation and analysis of “designer catalyst arrays”, nano-printed in a desired pattern on a solid support.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TA Engineering (General). Civil engineering (General) |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Cobaloximes , Carbon composites, Carbon, Hydrogen evolution reaction , Nanostructured materials | ||||||||||||
Journal or Publication Title: | Chemistry – A European Journal | ||||||||||||
Publisher: | Wiley | ||||||||||||
ISSN: | 1521-3765 | ||||||||||||
Official Date: | 6 December 2021 | ||||||||||||
Dates: |
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Volume: | 27 | ||||||||||||
Number: | 68 | ||||||||||||
Page Range: | pp. 16896-16903 | ||||||||||||
DOI: | 10.1002/chem.202102778 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Reuse Statement (publisher, data, author rights): | This is the peer reviewed version of the following article: Oswald, E., Gaus, A., Kund, J., Küllmer, M., Romer, J., Weizenegger, S., Ullrich, T., Mengele, A..K., Petermann, L., Leiter, R., Unwin, P..R., Kaiser, U., Rau, S., Kahnt, A., Turchanin, A., von Delius, M. and Kranz, C. (2021), Cobaloxime complex salts: synthesis, patterning on carbon nanomembranes and heterogeneous hydrogen evolution studies. Chem. Eur. J., which has been published in final form at https://doi.org/10.1002/chem.202102778. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited. | ||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||
Date of first compliant deposit: | 11 November 2021 | ||||||||||||
Date of first compliant Open Access: | 3 December 2021 | ||||||||||||
RIOXX Funder/Project Grant: |
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