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Increased Water Reduction Efficiency of Polyelectrolyte‐Bound Trimetallic [Ru,Rh,Ru] Photocatalysts in Air‐Saturated Aqueous Solutions
Author(s) -
Canterbury Theodore R.,
Arachchige Shamindri M.,
Moore Robert B.,
Brewer Karen J.
Publication year - 2015
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201506567
Subject(s) - aqueous solution , photocatalysis , chemistry , pyrazine , supramolecular chemistry , photochemistry , ligand (biochemistry) , quenching (fluorescence) , catalysis , inorganic chemistry , organic chemistry , molecule , fluorescence , biochemistry , physics , receptor , quantum mechanics
The groundbreaking use of polyelectrolytes to increase the efficiency of supramolecular photocatalysts in solar H 2 production schemes under aqueous aerobic conditions is reported. Supramolecular photocatalysts of the architecture [{(TL) 2 Ru(BL)} 2 RhX 2 ] 5+ (BL=bridging ligand, TL=terminal ligand, X=halide) demonstrate high efficiencies in deoxygenated organic solvents but do not function in air‐saturated aqueous solution because of the quenching of the metal‐to‐ligand charge‐transfer (MLCT) excited state under these conditions. The new photocatalytic system incorporates poly(4‐styrenesulfonate) (PSS) into aqueous solutions containing [{(bpy) 2 Ru(dpp)} 2 RhCl 2 ] 5+ (bpy=2,2′‐bipyridine, dpp=2,3‐bis(2‐pyridyl)pyrazine). PSS has a profound impact on the photocatalyst efficiency, increasing H 2 production over three times that of deoxygenated aqueous solutions alone. H 2 photocatalysis proceeds even under aerobic conditions for PSS‐containing solutions, an exciting consequence for solar hydrogen‐production research.