Covalent grafting of molecular catalysts on C 3 N x H y as robust, efficient and well-defined photocatalysts for solar fuel synthesis.

Autor: Windle CD; Department of Chemical Engineering UCL Torrington Place London WC1E 7JE UK junwang.tang@ucl.ac.uk., Wieczorek A; Department of Chemistry and Centre for Processable Electronics, Imperial College London, White City Campus London W12 0BZ UK., Xiong L; Department of Chemical Engineering UCL Torrington Place London WC1E 7JE UK junwang.tang@ucl.ac.uk., Sachs M; Department of Chemistry and Centre for Processable Electronics, Imperial College London, White City Campus London W12 0BZ UK., Bozal-Ginesta C; Department of Chemistry and Centre for Processable Electronics, Imperial College London, White City Campus London W12 0BZ UK., Cha H; Department of Chemistry and Centre for Processable Electronics, Imperial College London, White City Campus London W12 0BZ UK., Cockcroft JK; Department of Chemistry, University College London 20 Gordon Street London WC1H 0AJ UK., Durrant J; Department of Chemistry and Centre for Processable Electronics, Imperial College London, White City Campus London W12 0BZ UK., Tang J; Department of Chemical Engineering UCL Torrington Place London WC1E 7JE UK junwang.tang@ucl.ac.uk.
Jazyk: angličtina
Zdroj: Chemical science [Chem Sci] 2020 Jul 24; Vol. 11 (32), pp. 8425-8432. Date of Electronic Publication: 2020 Jul 24.
DOI: 10.1039/d0sc02986f
Abstrakt: The covalent attachment of molecules to 2D materials is an emerging area as strong covalent chemistry offers new hybrid properties and greater mechanical stability compared with nanoparticles. A nickel bis-aminothiophenol catalyst was grafted onto a range of 2D carbon nitrides (C 3 N x H y ) to form noble metal-free photocatalysts for H 2 production. The hybrids produce H 2 beyond 8 days with turnover numbers reaching 1360 based on nickel, a more than 3 fold higher durability than reported molecular catalyst-carbon nitride mixtures, and under longer wavelengths (>475 nm). Time-resolved spectroscopy reveals sub-microsecond electron transfer to the grafted catalyst, six orders of magnitude faster compared with similar reports of non-grafted catalysts. The photoelectrons on the catalyst have a ca. 1000 times longer half-time (7 ms) compared with bare carbon nitride (10 μs). The grafting strategy operates across a range of molecular catalyst-carbon nitride combinations, thus paving the way for robust efficient photocatalysts based on low-cost tunable components.
Competing Interests: There are no conflicts to declare.
(This journal is © The Royal Society of Chemistry.)
Databáze: MEDLINE
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