98%
921
2 minutes
20
A polystyrene-based chromophore-catalyst assembly (poly-2) has been synthesized and assembled at a mesoporous metal oxide photoanode. The assembly contains water oxidation catalyst centers based on [Ru(trpy) (phenq)] (Ru-Cat) and [Ru(bpy)] derivatives (Ru-C) as chromophores (trpy= 2,2';6,2″- terpyridine, phenq = 2-(quinol-8'-yl)-1,10-phenanthroline and bpy = 2,2'-bipyridine). The photophysical and electrochemical properties of the polychromophore-oxidation catalyst assembly were investigated in solution and at the surface of mesoporous metal oxide films. The layer-by-layer (LbL) method was utilized to construct multilayer films with cationic poly-2 and anionic poly(acrylic acid) (PAA) for light-driven photochemical oxidations. Photocurrent measurements of (PAA/poly-2) LbL films on mesoporous TiO demonstrate light-driven oxidation of phenol and benzyl alcohol in aqueous solution. Interestingly, illumination of (PAA/poly-2) LbL films on a fluorine doped SnO/TiO core/shell photoanode in aqueous solution gives rise to an initial photocurrent (∼18.5 μA·cm) that is in part ascribed to light driven water oxidation.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1021/acsami.7b05173 | DOI Listing |
Small
April 2025
Research Center for Photoenergy Harvesting & Conversion Technology (phct), Department of Energy and Materials Engineering, Dongguk University, Seoul, 04620, Republic of Korea.
Dye-sensitized photoelectrochemical cells (DSPECs) are efficient and sustainable approaches for hydrogen production via water splitting, driven by solar energy. Recent advancements have focused on enhancing the performance and stability of photoanodes, which are critical for efficient water oxidation. Herein discussed are the latest innovations including the development of metal-free organic sensitizers, improved chromophore-catalyst assemblies, and core-shell structures.
View Article and Find Full Text PDFDalton Trans
September 2024
Universidad de Buenos Aires, Facultad de Ciencias Exactas y Naturales, Departamento de Química Inorgánica, Analítica y Química Física, Pabellón 2, Ciudad Universitaria, C1428EHA, Buenos Aires, Argentina.
Chromophore-catalyst assemblies are interesting benchmark molecules for photocatalysis. We have prepared two examples of these assemblies and characterized their behaviour as catalysts for the water oxidation reaction. In the bimetallic complexes [Ru(tpy)(4,4'-X-bpy)(μ-CN)Ru(bda)(DMSO)](PF) (X = -H (1), -OCH (2), tpy = 2,2':6',2''-terpyridine, bpy = 2,2'-bipyridine, Hbda = 2,2'-bipyridine-6,6'-dicarboxylic acid and DMSO = (CH)SO), a Ru(II)-polypiridine chromophore {Ru(tpy)(4,4'-X-bpy)} is linked by a cyanide bridge to a {Ru(bda)} water oxidation catalyst.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2021
School of Chemistry and Biochemistry, School of Materials Science and Engineering, Center for Organic Photonics and Electronics, Georgia Tech Polymer Network, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.
Conjugated organic chromophores composed of linked donor (D) and acceptor (A) moieties have attracted considerable attention for photoelectrochemical applications. In this work, we compare the optoelectronic properties and photoelectrochemical performance of two D-A-D structural isomers with thiophene--carboxylic acid ( denotes 3 and 2 positions) derivatives and 2,1,3-benzothiadiazole as the D and A moieties, respectively. 5,5'-(Benzo[][1,2,5]thiadiazole-4,7-diyl)bis(thiophene-3-carboxylic acid), , and 5,5'-(benzo[][1,2,5]thiadiazole-4,7-diyl)bis(thiophene-2-carboxylic acid), , were employed in the study to understand how structural isomers affect surface attachments within chromophore-catalyst assemblies and their influence on charge-transfer dynamics.
View Article and Find Full Text PDFChemistry
December 2021
Dipartimento di Scienze Chimiche, Biologiche, Farmaceutiche ed Ambientali, Università di Messina, 98166, Messina, Italy.
The luminophore Ru(bpy) (dcbpy) (bpy=2,2'-bipyridine; dcbpy=4,4'-dicarboxy-2,2'-bipyridine) is covalently linked to a chitosan polymer; crosslinking by tripolyphosphate produced Ru-decorated chitosan fibers (NS-RuCh), with a 20 : 1 ratio between chitosan repeating units and Ru chromophores. The properties of the Ru compound are unperturbed by the chitosan structure, with NS-RuCh exhibiting the typical metal-to-ligand charge-transfer (MLCT) absorption and emission bands of Ru complexes. When crosslinks are made in the presence of IrO nanoparticles, such species are encapsulated within the nanofibers, thus generating the IrO ⊂NS-RuCh system, in which both Ru photosensitizers and IrO water oxidation catalysts are within the nanofiber structures.
View Article and Find Full Text PDFChemistry
June 2021
UNAM - National Nanotechnology Research Center Institute of Materials Science and Nanotechnology, Bilkent University, 06800, Ankara, Turkey.
The replacement of traditional ruthenium-based photosensitizers with low-cost and abundant iron analogs is a key step for the advancement of scalable and sustainable dye-sensitized water splitting cells. In this proof-of-concept study, a pyridinium ligand coordinated pentacyanoferrate(II) chromophore is used to construct a cyanide-based CoFe extended bulk framework, in which the iron photosensitizer units are connected to cobalt water oxidation catalytic sites through cyanide linkers. The iron-sensitized photoanode exhibits exceptional stability for at least 5 h at pH 7 and features its photosensitizing ability with an incident photon-to-current conversion capacity up to 500 nm with nanosecond scale excited state lifetime.
View Article and Find Full Text PDF