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Voltammetric and spectroscopic characterization of early intermediates in the Co(II)-polypyridyl-catalyzed reduction of water
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
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, Molecular Biomimetics.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
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2013 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 49, no 77, 8638-8640 p.Article in journal (Refereed) Published
Abstract [en]

Early intermediates of catalytic water reduction by a Co(II)-polypyridyl species have been characterized. Electrochemical detection of the Co(III)-hydride and time-resolved spectroscopic detection of the Co(I)-ligand intermediates provide an understanding of their reactivity in electrolytic or light-driven reduction of protons to hydrogen.

Place, publisher, year, edition, pages
2013. Vol. 49, no 77, 8638-8640 p.
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:uu:diva-208179DOI: 10.1039/c3cc44655gISI: 000323758900017OAI: oai:DiVA.org:uu-208179DiVA: diva2:651170
Available from: 2013-09-24 Created: 2013-09-24 Last updated: 2017-12-06
In thesis
1. Insight into Catalytic Intermediates Relevant for Water Splitting
Open this publication in new window or tab >>Insight into Catalytic Intermediates Relevant for Water Splitting
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Catalysis is an important part of chemistry. This is also reflected in the chemical industry where 85-90 % of all products are made catalytically. Also nature employs catalysts, i.e. enzymes, for its reactions.

To improve on the already existing catalysts one can learn a lot from nature which often uses earth-abundant elements in the enzymes which have also been optimized and finely tuned for billions of years. To gain a deeper understanding of both enzymatic and artificial catalysis one needs to investigate the mechanism of the catalytic process. But for very efficient catalysts with turnover frequencies of several thousand per second this is not easy, since an investigation of the mechanism involves resolving intermediates in the catalytic cycle. The intermediates in these instances are short-lived corresponding to their turnover frequencies. A maximum turnover frequency of 1,000 s-1 e.g. means that each catalyst goes through the whole catalytic cycle in 1 ms. Therefore time-resolved techniques are necessary that have a faster detection speed than the turnover frequency of the catalyst.

Flash photolysis is a spectroscopic technique with an instrument response function down to 10 ns.  Coupling this technique with mid-infrared probing yields an excellent detection system for probing different redox and protonation states of carbonyl metal complexes. Since many catalysts as well as natural enzymes involved in water splitting are metal carbonyl complexes this is an ideal technique to monitor the intermediates of these catalysts.

Chapter 3 covers the investigation of [FeFe] hydrogenases, enzymes that catalyze the reduction of protons to hydrogen in nature. Chapter 4 investigates the intermediates of biomimetic complexes, resembling the active site of natural [FeFe] hydrogenases. Chapter 5 covers the insights gained from investigating other catalysts which are also involved in water splitting and artificial photosynthesis.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2016. 81 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1359
Keyword
Catalysis, Artificial photosynthesis, Molecular biomimetics
National Category
Physical Chemistry
Research subject
Chemistry with specialization in Physical Chemistry; Chemistry with specialization in Chemical Physics
Identifiers
urn:nbn:se:uu:diva-281447 (URN)978-91-554-9526-8 (ISBN)
Public defence
2016-06-03, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
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Supervisors
Available from: 2016-05-11 Created: 2016-03-24 Last updated: 2016-06-01

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Singh, Wangkheimayum MarjitMirmohades, MohammadJane, Reuben T.White, Travis A.Hammarström, LeifThapper, AndersLomoth, ReinerOtt, Sascha

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