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Illuminating Benzothiadiazole : Mechanistic Insights into its Role in Fuel-Forming Reactions
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- Axelsson, Martin, 1993- (författare)
- Uppsala universitet,Fysikalisk kemi
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- Tian, Haining, 1983- (preses)
- Uppsala universitet,Fysikalisk kemi
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- Hammarström, Leif, 1964- (preses)
- Uppsala universitet,Fysikalisk kemi
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- ISBN 9789151318776
- Uppsala : Acta Universitatis Upsaliensis, 2023
- Engelska 90 s.
- Doktorsavhandling (övrigt vetenskapligt/konstnärligt)
Abstract
Ämnesord
Stäng
- Development and understanding of catalytic reactions involved in fuel formation are crucial to be able to make the energy transition into a sustainable future. One intriguing type of catalyst for these types of reactions is organic material catalysts, which combine some of the tunable nature of molecular catalysts with the scalability and robust nature of material catalysts. The understanding of the catalytic mechanisms in these types of materials is still a work in progress. In the last decade D-A type polymers have gotten a lot of attention as potential photocatalysts for fuel-forming reactions but currently, the mechanisms in which these reactions take place are very limited.This thesis focuses on the molecular unit benzothiadiazole (BT) and its role in catalytic fuel-forming reactions across various molecules and polymers. In paper I: The hydrogen evolution reaction (HER) is investigated on the small molecule 2,1,3-benzothiadiazole-4,7dicarbonitrile (BT). The study reveals that BTDN serves as an electrocatalyst for the HER. Some catalytic intermediates were identified spectroscopically and a catalytic mechanism was proposed.In papers II and III: Polymeric nanoparticles (Pdots) based on the polymer poly(9,9- dioctylfluorene-alt-2,1,3-benzothiadiazole (PFBT) were investigated for photocatalytic fuel-forming reactions. First, the HER was explored and it emphasised the significance of proton binding to the BT unit as a catalytic intermediate. It also showed that changing to basic conditions can quench the HER and make place for CO2 reduction to CO and that PFBT Pdots exhibit good selectivity in catalyzing this reaction.Finally, in Paper IV, the binding and reduction of CO2 on the molecule BTDN were investigated. It was shown that BTDN can bind CO2 in multiple reduced states and reduce it to CO and oxalate in a third reduction, albeit with seemingly low efficiencies.
Ämnesord
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Nyckelord
- Photocatalysis
- Electrocatalysis
- Renewable Energy
- Mechanistic Studies
- Cyclic Voltammetry
- Benzothiadiazole
Publikations- och innehållstyp
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