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Hydrogen evolution with CsPbBr3 perovskite nanocrystals under visible light in solution
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Department of Chemistry, Qena Faculty of Science, South Valley University, Qena, Egypt.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Institute of Physical Chemistry, Polish Academy of Sciences, Warsaw, Poland.ORCID iD: 0000-0003-2124-9510
2018 (English)In: MATERIALS TODAY COMMUNICATIONS, ISSN 2352-4928, Vol. 16, p. 90-96Article in journal (Refereed) Published
Abstract [en]

Direct proton photo-reduction to molecular hydrogen with a lead-halide perovskite photosystem is presented. The concept uses CsPbBr3 nanocrystals and Ru@TiO2 nanoparticles as light harvesters and catalyst, respectively. The photo-system attains charge transfer from donor to acceptor via collision events, established via static and ultrafast spectroscopy. The photo-system exhibits a photon-to-hydrogen efficiency of ca. 0.4%, a respectable efficiency for a system relying on effective collisions for the transference of electrons.

Place, publisher, year, edition, pages
2018. Vol. 16, p. 90-96
Keywords [en]
Inorganic perovskites nanocrystals, H-2 evolution, Ultrafast spectroscopy, Charge transfer via collision
National Category
Materials Chemistry Physical Chemistry Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-364171DOI: 10.1016/j.mtcomm.2018.05.001ISI: 000443035000012OAI: oai:DiVA.org:uu-364171DiVA, id: diva2:1261042
Funder
Swedish Research CouncilStiftelsen Olle Engkvist ByggmästareAvailable from: 2018-11-06 Created: 2018-11-06 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.Sá, Jacinto

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