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Dynamics and Photochemical H-2 Evolution of Dye-NiO Photocathodes with a Biomimetic FeFe-Catalyst
Department of Chemistry—Ångström Laboratory, Uppsala University.
Luleå University of Technology, Department of Engineering Sciences and Mathematics, Material Science.ORCID iD: 0000-0002-7893-7405
Department of Chemistry—Ångström Laboratory, Uppsala University.
Department of Chemistry—Ångström Laboratory, Uppsala University.
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Number of Authors: 62016 (English)In: ACS Energy Letters, ISSN 2380-8195, Vol. 1, no 6, p. 1106-1111Article in journal (Refereed) Published
Abstract [en]

Mesoporous NiO films were cosensitized with a coumarin 343 dye and a proton reduction catalyst of the [Fe-2(CO)(6)(bdt)] (bdt = benzene-1,2-dithiolate) family. Femtosecond ultraviolet visible transient absorption experiments directly demonstrated subpicosecond hole injection into NiO from excited dyes followed by rapid (t(50%) similar to 6 ps) reduction of the catalyst on the surface with similar to 70% yield. The reduced catalyst was long-lived (2 mu s to 20 ms), which may allow protonation and a second reduction step of the catalyst to occur. A photo electrochemical device based on this photocathode produced H-2 with a Faradaic efficiency of similar to 50%. Fourier transform infrared spectroscopy and gas chromatography experiments demonstrated that the observed device deterioration with time was mainly due to catalyst degradation and desorption from the NiO surface. The insights gained from these mechanistic studies, regarding development of dye-catalyst cosensitized photocathodes, are discussed.

Place, publisher, year, edition, pages
2016. Vol. 1, no 6, p. 1106-1111
National Category
Other Physics Topics
Research subject
Experimental Physics
Identifiers
URN: urn:nbn:se:ltu:diva-61410DOI: 10.1021/acsenergylett.6b00506ISI: 000390086400005OAI: oai:DiVA.org:ltu-61410DiVA, id: diva2:1064602
Note

Validerad; 2017; Nivå 2; 2017-01-12 (andbra)

Available from: 2017-01-12 Created: 2017-01-12 Last updated: 2019-04-19Bibliographically approved
In thesis
1. Advanced Metal Oxide Semiconductors for Solar Energy Harvesting and Solar Fuel Production
Open this publication in new window or tab >>Advanced Metal Oxide Semiconductors for Solar Energy Harvesting and Solar Fuel Production
2017 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

Increasing energy consumption and its environmental impacts make it necessary to look for alternative energy sources. Solar energy as huge energy source which is able to cover the terms sustainability is considered as a favorable alternative. Solar cells and solar fuels are two kinds of technologies, which make us able to harness solar energy and convert it to electricity and/or store it chemically.

Metal oxide semiconductors (MOSs) have a major role in these devices and optimization of their properties (composition, morphology, dimensions, crystal structure) makes it possible to increase the performance of the devices. The light absorption, charge carriers mobility, the time scale between charge injection, regeneration and recombination processes are some of the properties critical to exploitation of MOSs in solar cells and solar fuel technology.

In this thesis, we explore two different systems. The first one is a NiO mesoporous semiconductor photocathode sensitized with a biomimetic Fe-Fe catalyst and a coumarin C343 dye, which was tested in a solar fuel device to produce hydrogen. This system is the first solar fuel device based on a biomimetic Fe-Fe catalyst and it shows a Faradic efficiency of 50% in hydrogen production. Cobalt catalysts have higher Faradic efficiency but their performance due to hydrolysis in low pH condition is limited. The second one is a photoanode based on the nanostructured hematite/magnetite film, which was tested in a photoelectrochemical cell. This hybrid electrode improved the photoactivity of the photoelectrochemical cell for water splitting. The main mechanism for the improvement of the functional properties relies with the role of the magnetite phase, which improves the charge carrier mobility of the composite system, compared to pure hematite, which acts as good light absorber semiconductor.

By optimizing the charge separation and mobility of charge carriers of MOSs, they can be a promising active material in solar cells and solar fuel devices due to their abundance, stability, non-toxicity, and low-cost. The future work will be focused on the use of nanostructured MOSs in all-oxide solar cell devices. We have already obtained some preliminary results on 1-dimensional heterojunctions, which we report in Chapter 3.3. While they are not conclusive, they give an idea about the future direction of the present research. 

Place, publisher, year, edition, pages
Luleå: Luleå University of Technology, 2017
Series
Licentiate thesis / Luleå University of Technology, ISSN 1402-1757
Keywords
Photovoltaic, Semiconductors, Photoelectrochemical cell, Solar fuel, Water splitting, Hydrogen evolution, Oxygen evolution
National Category
Other Physics Topics
Research subject
Experimental Physics
Identifiers
urn:nbn:se:ltu:diva-64922 (URN)978-91-7583-979-0 (ISBN)978-91-7583-980-6 (ISBN)
Presentation
2017-11-08, E231, Luleå, 10:00 (English)
Opponent
Supervisors
Funder
VINNOVA, 224320
Available from: 2017-09-26 Created: 2017-09-26 Last updated: 2018-10-22Bibliographically approved
2. Advanced Nanostructured Transition Metal Oxide Semiconductors for Solar Energy Applications
Open this publication in new window or tab >>Advanced Nanostructured Transition Metal Oxide Semiconductors for Solar Energy Applications
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Avanceradenanostrukturerade halvledare av övergångsmetalloxid för solenergiapplikationer
Abstract [en]

Increasing energy consumption and its environmental impacts make it necessary to look for alternative energy sources. Solar energy as huge energy source that can cover the terms sustainability is considered as a favorable alternative. Optoelectronic devices like solar cells and photoelectrochemical cells are in very high interest to provide the energy that we need. They can convert solar energy, as a sustainable energy source, to electricity and fuel. Transition metal oxides (TMOs) due to high chemical stability, abundance, facile production and low cost are favorable materials to be used in these optoelectronic applications. In TMOs, d orbitals electrons contribute in forming bonds that gives special magnetic, electronic and geometric characteristics to these materials. They can be synthesized with different types of chemical and physical deposition methods.

The electronic properties of TMOs varies from metallic characteristics to electrical insulators. Transition metal oxide semiconductors (TMOSs) are mostly used in optoelectronic devices. Tuning the properties of TMOSs like, composition, morphology, dimensions, crystal structure, improves the performance of the optoelectronic devices. The light absorption, charge carrier mobility, the time scale between charge injection, regeneration and recombination processes are some of the properties critical to exploitation of TMOSs in solar cells and solar fuel technology.

In this thesis, we explore the use of nanostructured TMOSs in all-oxide solar cells, photodetectors and photoelectrochemical cells. 1-dimentional heterojunctions of n-type transparent semi-conductive metal oxides (ZnO and TiO2) in conjunction to p-type light absorbing semi-conductive metal oxides (Cu2O and Co3O4) have been tested in all-oxide photodetectors and solar cells.  It is shown that the 1-dimentional nanostructured geometry (nanowires, nanotubes) improves the charge separation and charge transport properties. Increasing the surface to volume aspect ratio in nanowires and nanotubes improves the light absorption compare to the thin film geometry. Our ZnO-Cu2O core-shell nanowire photodetector is the fastest visible light photodetector reported till now. Mesoporous NiO photocathode, sensitized with a biomimetic FeFe-catalyst and coumarin C343 dye, was tested in a photoelectrochemical cell for hydrogen production. This system is the first solar fuel device based on a biomimetic FeFe-catalyst and it shows a Faradic efficiency of 50% in hydrogen production. Cobalt catalysts have higher Faradic efficiency but their performance due to hydrolysis in low pH condition is limited. Nanostructured hematite/magnetite film as a photoanode was tested in a photoelectrochemical cell for water splitting. This hybrid electrode improved the photoactivity of the photoelectrochemical cell for water splitting. The main mechanism for the improvement of the functional properties relies with the role of the magnetite phase, which improves the charge carrier mobility of the composite system, compared to pure hematite, which acts as good light absorbing semiconductor.

Place, publisher, year, edition, pages
Luleå: Luleå University of Technology, 2019
Series
Doctoral thesis / Luleå University of Technology 1 jan 1997 → …, ISSN 1402-1544
Keywords
Metal Oxide, Photovoltaic, Semiconductors, Self-powered photodetectors, Photoelectrochemical cell, Solar fuel, Water splitting
National Category
Materials Engineering
Research subject
Experimental Physics
Identifiers
urn:nbn:se:ltu:diva-73709 (URN)978-91-7790-366-6 (ISBN)978-91-7790-367-3 (ISBN)
Public defence
2019-06-14, E632, Luleå University of Technology, Luleå, 10:00 (English)
Opponent
Supervisors
Funder
Vinnova, 224320
Available from: 2019-04-23 Created: 2019-04-19 Last updated: 2019-05-22Bibliographically approved

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