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Control the O-O bond formation pathways by immobilizing molecular catalysts on glassy carbon via electrochemical polymerization
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.ORCID iD: 0000-0003-3455-0855
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.ORCID iD: 0000-0003-1662-5817
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Molecular water oxidation catalysts Ru-bda (1) and Ru-pda (2) are electrochemically polymerized on glassy carbon (GC) electrodes. Reaction orders and kinetic isotope effects (KIE) of the corresponding electrodes are studied. Results indicate that poly-1@GC goes through a radical coupling pathway. By adding poly-styrene (PSt) as a “blocking unit” in the poly-1, the radical coupling process of Ru-bda is blocked, and poly-1+PSt@GC catalyzes water oxidation through the water nucleophilic attack pathway. In comparison, catalyst 2, which oxidizes water via water nucleophilic attack path in homogeneous systems, goes through a radical coupling pathway as well when 2 is polymerized on glassy carbon (poly-2@GC).

Keyword [en]
kinetics
National Category
Other Chemistry Topics
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-181103OAI: oai:DiVA.org:kth-181103DiVA: diva2:898688
Funder
Swedish Energy Agency, B61649
Note

QS 2016

Available from: 2016-01-29 Created: 2016-01-29 Last updated: 2016-02-01Bibliographically approved
In thesis
1. Design of Water Splitting Devices via Molecular Engineering
Open this publication in new window or tab >>Design of Water Splitting Devices via Molecular Engineering
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Converting solar energyto fuels such as hydrogen by the reaction of water splitting is a promising solution for the future sustainable energy systems. The theme of this thesis is to design water splitting devices via molecular engineering; it concerns the studies of both electrochemical-driven and photo-electrochemical driven molecular functional devices for water splitting.

The first chapter presents a general introduction about Solar Fuel Conversion. It concerns molecular water splitting catalysts, light harvesting materials and fabrication methods of water splitting devices.

The second chapter describes an electrode by immobilizing a molecular water oxidation catalyston carbon nanotubes through the hydrophobic interaction. This fabrication method is corresponding to the question: “How to employ catalysts in functional devices without affecting their performances?”

In the third chapter, molecular water oxidation catalysts were successfully immobilized on glassy carbon electrode surface via electrochemical polymerization method. The O-O bond formation pathways of catalysts on electrode surfaces were studied. This kinetic studyis corresponding to the question: “How to get kinetic information of RDS whena catalyst is immobilized on the electrode surface?”

Chapter four explores molecular water oxidation catalysts immobilized on dye-sensitized TiO2 electrodeand Fe2O3 semiconductor electrode via different fabrication methods. The reasons of photocurrent decay are discussed and two potential solutions are provided. These studies are corresponding to the question: “How to improvethe stability of photo-electrodes?”

Finally, in the last chapter, two novel Pt-free Z-schemed molecular photo-electrochemical cells with both photoactive cathode and photoactive anode for visible light driven water splitting driven were demonstrated. These studies are corresponding to the question: “How to utilizethe concept of Z-schemein photosynthesis to fabricate Pt-free molecular based PEC cells?

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2016. 92 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2016:6
Keyword
electrochemical-driven water splitting, artificial photosynthesis, molecular catalysts
National Category
Other Chemistry Topics
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-181107 (URN)978-91-7595-841-5 (ISBN)
Public defence
2016-02-26, F3, Lindstedtsvägen 26, KTH, Stockholm., 10:00 (English)
Opponent
Supervisors
Funder
Swedish Energy AgencySwedish Research CouncilKnut and Alice Wallenberg Foundation
Note

QC 20160129

Available from: 2016-01-29 Created: 2016-01-29 Last updated: 2016-01-29Bibliographically approved

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