Dye-sensitized photo-oxidation of enzymes.
Ontology highlight
ABSTRACT:
SUBMITTER: Tsai CS
PROVIDER: S-EPMC1144570 | biostudies-other | 1985 Jan
REPOSITORIES: biostudies-other
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Project description:Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO2 grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm-2 was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of a buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor-electrocatalyst junction behaviors in the presence of a poor semiconducting material.
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Project description:This work reports an aqueous dye-sensitized photoelectrochemical cell (DSPEC) capable of oxidizing glycerol (an archetypical biobased compound) coupled with H2 production. We employed a mesoporous TiO2 photoanode sensitized with the high potential thienopyrroledione-based dye AP11, encased in an acetonitrile-based redox-gel that protects the photoanode from degradation by aqueous electrolytes. The use of the gel creates a biphasic system with an interface at the organic (gel) electrode and aqueous anolyte. Embedded in the acetonitrile gel is 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), acting as both a redox-mediator and a catalyst for oxidative transformations. Upon oxidation of TEMPO by the photoexcited dye, the in situ generated TEMPO+ shuttles through the gel to the acetonitrile-aqueous interface, where it acts as an oxidant for the selective conversion of glycerol to glyceraldehyde. The introduction of the redox-gel layer affords a 10-fold increase in the conversion of glycerol compared to the purely aqueous system. Our redox-gel protected photoanode yielded a stable photocurrent over 48 hours of continuous operation, demonstrating that this DSPEC is compatible with alkaline aqueous reactions.
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Project description:Splitting one high-energy photon into two lower energy photons through downconversion has been demonstrated for a variety of combinations of rare earth (RE) ions. However, the low absorption cross section of RE3+ 4f-4f transitions hampers practical application. Therefore, enhancing the absorption by sensitization is crucial. We demonstrate efficient dye-sensitized downconversion using a strong blue/UV absorbing Coumarin dye to sensitize downconversion of the Pr3+-Yb3+ couple in NaYF4 nanocrystals (NCs). Luminescence spectra and lifetime measurements reveal Förster resonant energy transfer (FRET) from Coumarin to Pr3+ in NaYF4:Pr3+Yb3+ NCs, followed by downconversion, resulting in Yb3+ IR emission with ∼30 times enhancement. The present study demonstrates the feasibility of dye-sensitized downconversion as a promising strategy to engineer strongly absorbing downconversion NCs to enhance the efficiency of photovoltaic cells.
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Project description:In the development of photoelectrochemical cells for water splitting or CO2 reduction, a major challenge is O2 evolution at photoelectrodes that, in behavior, mimic photosystem II. At an appropriate semiconductor electrode, a water oxidation catalyst must be integrated with a visible light absorber in a stable half-cell configuration. Here, we describe an electrode consisting of a light absorber, an intermediate electron donor layer, and a water oxidation catalyst for sustained light driven water oxidation catalysis. In assembling the electrode on nanoparticle SnO2/TiO2 electrodes, a Ru(II) polypyridyl complex was used as the light absorber, NiO was deposited as an overlayer, and a Ru(II) 2,2'-bipyridine-6,6'-dicarboxylate complex as the water oxidation catalyst. In the final electrode, addition of the NiO overlayer enhanced performance toward water oxidation with the final electrode operating with a 1.1 mA/cm2 photocurrent density for 2 h without decomposition under one sun illumination in a pH 4.65 solution. We attribute the enhanced performance to the role of NiO as an electron transfer mediator between the light absorber and the catalyst.
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Project description:This work reports a dye-sensitized photoelectrochemical cell (DSPEC) that couples redox-mediated light-driven oxidative organic transformations to reductive hydrogen (H2 ) formation. The DSPEC photoanode consists of a mesoporous anatase TiO2 film on FTO (fluorine-doped tin oxide), sensitized with the thienopyrroledione-based dye AP11, while H2 was formed at a FTO-Pt cathode. Irradiation of the dye-sensitized photoanode transforms 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) to the oxidized TEMPO (TEMPO+ ), which acts as a chemical oxidant for the conversion of benzyl alcohol. The TEMPO0/+ couple, previously used as redox mediator in DSSC, mediates efficient electron transfer from the organic substrate to the photo-oxidized dye. A DSPEC photoreactor was designed that allows in situ monitoring the reaction progress by infrared spectroscopy and gas chromatography. Sustained light-driven oxidation of benzyl alcohol to benzaldehyde within the DSPEC photoreactor, using of TEMPO as mediator, demonstrated the efficiency of the device, with a photocurrent of 0.4 mA cm-2 , approaching quantitative Faradaic efficiency and exhibiting excellent device stability.
| S-EPMC7839774 | biostudies-literature
Project description:Understanding and controlling the properties of water-splitting assemblies in dye-sensitized photoelectrosynthesis cells is a key to the exploitation of their properties. We demonstrate here that, following surface loading of a [Ru(bpy)3]2+ (bpy = 2,2'-bipyridine) chromophore on nanoparticle electrodes, addition of the molecular catalysts, Ru(bda)(L)2 (bda = 2,2'-bipyridine-6,6'-dicarboxylate) with phosphonate or pyridyl sites for water oxidation, gives surfaces with a 5:1 chromophore to catalyst ratio. Addition of the surface-bound phosphonate derivatives with L = 4-pyridyl phosphonic acid or diethyl 3-(pyridin-4-yloxy)decyl-phosphonic acid, leads to well-defined surfaces but, following oxidation to Ru(III), they undergo facile, on-surface dimerization to give surface-bound, oxo-bridged dimers. The dimers have a diminished reactivity toward water oxidation compared to related monomers in solution. By contrast, immobilization of the Ru-bda catalyst on TiO2 with the 4,4'-dipyridyl anchoring ligand can maintain the monomeric structure of catalyst and gives relatively stable photoanodes with photocurrents that reach to 1.7 mA cm-2 with an optimized, applied bias photon-to-current efficiency of 1.5%.
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Project description:Styryl (FM) dyes have been used for more than two decades to investigate exo- and endocytosis in conventional synapses. However, they are difficult to use in the inner hair cells of the auditory pathway (IHCs), as FM dyes appear to penetrate through mechanotransducer channels into the cytosol of IHCs, masking endocytotic uptake. To solve this problem we applied to IHCs the FM dye photo-oxidation technique, which renders the dyes into electron microscopy markers. Photo-oxidation allowed the unambiguous identification of labeled organelles, despite the presence of FM dye in the cytosol. This enabled us to describe the morphologies of several organelles that take up membrane in IHCs, both at rest and during stimulation. At rest, endosome-like organelles were detected in the region of the cuticular plate. Larger tubulo-cisternal organelles dominated the top and nuclear regions. Finally, the basal region, where the IHC active zones are located, contained few labeled organelles. Stimulation increased significantly membrane trafficking in the basal region, inducing the appearance of labeled vesicles and cistern-like organelles. The latter were replaced by small, synaptic-like vesicles during recovery after stimulation. In contrast, no changes in membrane trafficking were induced by stimulation in the cuticular plate region or in the top and nuclear regions. We conclude that synaptic vesicle recycling takes place mostly in the basal region of the IHCs. Other organelles participate in abundant constitutive membrane trafficking throughout the rest of the IHC volume.
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Project description:Acetylene-black paste without a light scattering layer was applied to meso-porous TiO2 photo-electrode films with a crystalline framework, a low residual carbon, and a tunable morphological pore size. The thermal-treated TiO2 photo-electrode films had an increased acetylene-black concentration with an increase in artificial pores and a decrease in residual carbon. The performance of dye-sensitized solar cells (DSSCs) was enhanced by the use of the TiO2 photo-anode pastes at various acetylene-black concentrations. The photo-conversion efficiency of the DSSCs using TiO2 photo-electrode films with 1.5 wt% acetylene-black was enhanced from 7.98 (no acetylene-black) to 9.75% without the integration of a light- scattering layer.
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Project description:BackgroundDye-sensitized solar cells (DSSCs) have garnered a lot of attention in recent years. The solar energy to power conversion efficiency of a DSSC is influenced by various components of the cell such as the dye, electrolyte, electrodes and additives among others leading to varying experimental configurations. A large number of metal-based and metal-free dye sensitizers have now been reported and tools using such data to indicate new directions for design and development are on the rise.DescriptionDSSCDB, the first of its kind dye-sensitized solar cell database, aims to provide users with up-to-date information from publications on the molecular structures of the dyes, experimental details and reported measurements (efficiencies and spectral properties) and thereby facilitate a comprehensive and critical evaluation of the data. Currently, the DSSCDB contains over 4000 experimental observations spanning multiple dye classes such as triphenylamines, carbazoles, coumarins, phenothiazines, ruthenium and porphyrins.ConclusionThe DSSCDB offers a web-based, comprehensive source of property data for dye sensitized solar cells. Access to the database is available through the following URL: www.dyedb.com .
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Project description:From atomic level to understand the cluster-size-dependant behavior of dye-sensitized photocatalysts is very important and helpful to design new photocatalytic materials. Although the relationship between the photocatalytic behaviors and particles' size/shape has been widely investigated by theoretical scientists, the experimental evidences are much less. In this manuscript, we successfully synthesized three new ruthenium dye-sensitized polyoxometalates (POM-n, n relate to different size clusters) with different-sized POM clusters. Under visible-light illumination, all three complexes show the stable O2 evolution with the efficient order POM-3 > POM-2 > POM-1. This cluster-size-dependent catalytic behavior could be explained by the different numbers of M = Ot (terminal oxygen) bonds in each individual cluster because it is well-known that Mo = Ot groups are the catalytically active sites for photooxidation reaction. The proposed mechanism of water oxidation for the dye-sensitized POMs is radical reaction process. This research could open up new perspectives for developing new POM-based WOCs.
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