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Organic heterojunction photocathodes for optimized photoelectrochemical hydrogen peroxide production
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-8478-4663
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0002-0280-8017
2018 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 48, p. 24709-24716Article in journal (Refereed) Published
Abstract [en]

Solar-to-chemical conversion of sunlight into hydrogen peroxide as a chemical fuel is an emerging carbon-free sustainable energy strategy. The process is based on the reduction of dissolved oxygen to hydrogen peroxide. Only limited amounts of photoelectrode materials have been successfully explored for photoelectrochemical production of hydrogen peroxide. Herein we detail approaches to produce robust organic semiconductor photocathodes for peroxide evolution. They are based on evaporated donor-acceptor heterojunctions between phthalocyanine and tetracarboxylic perylenediimide, respectively. These small molecules form nanocrystalline films with good operational stability and high surface area. We discuss critical parameters which allow fabrication of efficient devices. These photocathodes can support continuous generation of high concentrations of peroxide with faradaic efficiency remaining at around 70%. We find that an advantage of the evaporated heterojunctions is that they can be readily vertically stacked to produce tandem cells which produce higher voltages. This feature is desirable for fabricating two-electrode photoelectrochemical cells. Overall, the photocathodes presented here have the highest performance reported to date in terms of photocurrent for peroxide production. These results offer a viable method for peroxide photosynthesis and provide a roadmap of strategies that can be used to produce photoelectrodes with even higher efficiency and productivity.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2018. Vol. 6, no 48, p. 24709-24716
National Category
Other Chemical Engineering
Identifiers
URN: urn:nbn:se:liu:diva-153662DOI: 10.1039/c8ta08151dISI: 000453550700005OAI: oai:DiVA.org:liu-153662DiVA, id: diva2:1276250
Note

Funding Agencies|Knut and Alice Wallenberg Foundation; Wallenberg Centre for Molecular Medicine at Linkoping University; Vinnova within the framework of Treesearch.se

Available from: 2019-01-07 Created: 2019-01-07 Last updated: 2020-02-25
In thesis
1. Organic electronic materials for hydrogen peroxide production
Open this publication in new window or tab >>Organic electronic materials for hydrogen peroxide production
2020 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Hydrogen peroxide (H2O2) is an important oxidant, used in various fields of industry, such as paper manufacturing, production of polymers, detergents, and cosmetics. Considering that the molecule degrades only to H2O and O2, it is regarded as a green chemical. Unfortunately, the incumbent method of H2O2 synthesis, based on anthraquinone oxidation, although efficient, is not environmentally friendly, as it requires fossil fuels and significant energy input. Therefore, there are efforts underway to reduce the ecological impact of hydrogen peroxide production. Some of the most promising approaches involve catalytic reduction of O2 to H2O2 in an aqueous environment. This can be coupled with water oxidation. As the required energy could be delivered in different ways, hydrogen peroxide synthesis can be achieved by electrocatalysis, photoelectrocatalysis, or photocatalysis.

This thesis explores the possibility of using organic electronic materials as catalysts for H2O2 evolution in oxygenated water solutions. Organic electronics is a field of materials science focused on conducting and semiconducting organic molecules. These materials offer many possible advantages, related to low cost, flexibility, and good optoelectronic properties. Huge progress in the field over the last years led to their commercial applications in e.g. organic light emitting diodes and photovoltaics. Only very recently have organic electronics begun to be considered from the point of view of catalysis.

In the first two papers, we investigate electrocatalytic activity of an organic pigment (PTCDI) and a conducting polymer (PEDOT) towards oxygen reduction to hydrogen peroxide. Both types of catalysts are chemically stable and able to operate in a wide pH range. In paper 3, we demonstrate that H2O2-evolving photocathodes can be based on an organic PN heterojunction, giving devices of a record-breaking performance. In the first part of paper 4, the same concept was tested for a naturally-occurring semiconductor, eumelanin, leading to a first report of photoelectrocatalytic properties of this material. In the second part of paper 4, as well as in papers 5 and 6, we explore, respectively, photochemical hydrogen peroxide synthesis with eumelanin, organic semiconductors, and organic dyes. We show that the photostability of catalysts is higher for materials with low-lying HOMO level and it can be increased by an addition of a reducing agent to the reaction system. Our findings prove that already existing organic electronic materials can be successfully applied in H2O2 evolution for environmentally friendly chemical synthesis, suggesting their use in harvesting of solar energy and in situ generation of hydrogen peroxide for biomedical applications.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2020. p. 92
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2037
Keywords
hydrogen peroxide, catalysis, organic materials, electronics
National Category
Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-163895 (URN)978-91-7929-939-2 (ISBN)
Public defence
2020-03-30, K1, Kåkenhus, Campus Norrköping, Norrköping, 10:15 (English)
Opponent
Supervisors
Funder
Knut and Alice Wallenberg Foundation, WCMM-LiU
Available from: 2020-02-25 Created: 2020-02-25 Last updated: 2020-02-25Bibliographically approved

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