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Nano-hybrid plasmonic photocatalyst for hydrogen production at 20% efficiency
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-05508000 Sao Paulo, Brazil.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
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2017 (English)In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 7, article id 8670Article in journal (Refereed) Published
Abstract [en]

The efficient conversion of light energy into chemical energy is key for sustainable human development. Several photocatalytic systems based on photovoltaic electrolysis have been used to produce hydrogen via water reduction. However, in such devices, light harvesting and proton reduction are carried separately, showing quantum efficiency of about 10–12%. Here, we report a nano-hybrid photocatalytic assembly that enables concomitant reductive hydrogen production and pollutant oxidation with solar-to-fuel efficiencies up to 20%. The modular architecture of this plasmonic material allows the fine-tuning of its photocatalytic properties by simple manipulation of a reduced number of basic components.

Place, publisher, year, edition, pages
2017. Vol. 7, article id 8670
National Category
Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
URN: urn:nbn:se:uu:diva-328630DOI: 10.1038/s41598-017-09261-7ISI: 000407864400051OAI: oai:DiVA.org:uu-328630DiVA, id: diva2:1136628
Funder
The Swedish Foundation for International Cooperation in Research and Higher Education (STINT), IB2015-6474Available from: 2017-08-28 Created: 2017-08-28 Last updated: 2018-12-17Bibliographically approved
In thesis
1. Accumulative Charge Separation in Photocatalysis: From Molecules to Nanoparticles
Open this publication in new window or tab >>Accumulative Charge Separation in Photocatalysis: From Molecules to Nanoparticles
2019 (English)Doctoral thesis, comprehensive summary (Other academic) [Artistic work]
Abstract [en]

Photochemical energy conversion into solar fuel involves steps of light absorption, charge separation and catalysis. Nature has taught us that the effective accumulation of redox equivalents and charge separation are the key steps in sunlight conversion. The focus of this thesis is to unveil photophysical and photochemical processes that lead to accumulative charge separation. The optimization of electron transfer process will be held by minimization of losses via recombination, and extension of the lifetime of the charge separated state by usage of the electron relay.

The goal is to couple light induced electron transfer process with the multi-electron catalytic process of hydrogen evolution. In this regard, light harvesters (molecules, metal nanostructures) that generate at least two electrons per absorbed photon will be studied. Additionally, semiconductors that generate long-lived charge separated states are utilized to accumulate several redox equivalents necessary for hydrogen evolution.

The hybrid systems produced by the combination of the advantageous properties of molecules, semiconductors, and metal nanoparticles are under the scope of investigation. Metal nanoparticles are advantageous because of their high absorption cross-section. The molecular linkers provide control and flexibility in tuning the connection between the light absorber and the electron relay. Semiconductor nanoparticles offer the desired charge separation properties via prolonging the lifetime sufficiently to perform photocatalysis.

The detailed understanding, investigation and development of the hybrid systems is at the heart of the progress of photochemical solar fuel production.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2019. p. 88
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1759
Keywords
Accumulative charge separation, Electron transfer, Plasmon dynamics, Time-resolved spectroscopy, Photocatalysis.
National Category
Chemical Sciences
Research subject
Chemistry with specialization in Physical Chemistry
Identifiers
urn:nbn:se:uu:diva-369930 (URN)978-91-513-0543-1 (ISBN)
Public defence
2019-02-22, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2019-01-23 Created: 2018-12-17 Last updated: 2019-02-18

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Pavliuk, Mariia V.Fernandes, Daniel L. A.Rocha, IgorHattori, YocefuSá, Jacinto

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