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Dye activation of heterogeneous Copper(II)-Species for visible light driven hydrogen generation

  • Heterogeneous Cu catalysts are widely used in photocatalytic hydrogen generation. The typical working mode includes the transfer of photo-induced charges from a semiconductor to CuO which itself is reduced to Cu2O to initiate the catalytic cycle. In this contribution a photosensitizer (dye), excited by visible light absorption, was used to transfer an electron to the CuO which after reduction catalyzes the water reduction to hydrogen. Several copper(II)-catalysts on high surface silica were prepared by impregnation or precipitation and applied in photocatalytic water reduction. The best catalyst CuO(Cl0.1)/SiO2, synthesized via incipient wetness impregnation of CuCl2 in MCM-41 and a following precipitation with NaOH, achieved a 6 times higher activity (1702 mmol h-1 g-1) compared to a previously investigated copper system (280 mmol h-1 g-1 for CuI) under the same reaction conditions. All materials were fully characterized by XRD, TEM and N2 sorption and further by magnetic resonanceHeterogeneous Cu catalysts are widely used in photocatalytic hydrogen generation. The typical working mode includes the transfer of photo-induced charges from a semiconductor to CuO which itself is reduced to Cu2O to initiate the catalytic cycle. In this contribution a photosensitizer (dye), excited by visible light absorption, was used to transfer an electron to the CuO which after reduction catalyzes the water reduction to hydrogen. Several copper(II)-catalysts on high surface silica were prepared by impregnation or precipitation and applied in photocatalytic water reduction. The best catalyst CuO(Cl0.1)/SiO2, synthesized via incipient wetness impregnation of CuCl2 in MCM-41 and a following precipitation with NaOH, achieved a 6 times higher activity (1702 mmol h-1 g-1) compared to a previously investigated copper system (280 mmol h-1 g-1 for CuI) under the same reaction conditions. All materials were fully characterized by XRD, TEM and N2 sorption and further by magnetic resonance and X-ray methods EPR, ASAXS and XAS. In situ measurements evidenced a reduction of the initial Cu(II)-species, which confirms the (proposed) photocatalytic mechanism.zeige mehrzeige weniger

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Autor*innen:S. Kreft, Jörg RadnikORCiD, G. Agostini, M.-M. Pohl, E. Gericke, Armin Hoell, M. Beller, H. Junge, S. Wohlrab
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):International Journal of Hydrogen Energy
Jahr der Erstveröffentlichung:2019
Organisationseinheit der BAM:6 Materialchemie
6 Materialchemie / 6.1 Oberflächen- und Dünnschichtanalyse
Verlag:Elsevier Ltd.
Jahrgang/Band:44
Ausgabe/Heft:53
Erste Seite:28409
Letzte Seite:28420
DDC-Klassifikation:Naturwissenschaften und Mathematik / Chemie / Analytische Chemie
Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Angewandte Physik
Freie Schlagwörter:CuO nanoparticles; Hydrogen generation; Molecular sieves
Themenfelder/Aktivitätsfelder der BAM:Chemie und Prozesstechnik
Energie
DOI:10.1016/j.ijhydene.2019.04.006
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:28.10.2019
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:05.12.2019
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