Catalyst-Free Synthesis of Robust Covalent Polymer Network Semiconducting Films and Application in Photoelectrochemical Water Splitting
Liang Yao a, Kevin Sivula a
a Ecole Polytechnique Federale de Lausanne (EPFL), Lausanne, Switzerland
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#SolFuel19. Solar Fuel Synthesis: From Bio-inspired Catalysis to Devices
Berlin, Germany, 2019 November 3rd - 8th
Organizers: Roel van de Krol and Erwin Reisner
Oral, Liang Yao, presentation 155
DOI: https://doi.org/10.29363/nanoge.nfm.2019.155
Publication date: 18th July 2019

Photoelectrochemical (PEC) water splitting is an enticing approach to directly convert solar energy into a chemical commodity like hydrogen paving the way for a sustainable carbon-neutral society. So far, discovering efficient, robust and cheap materials to drive solar water splitting stands out as the main challenge in this field.[1] Organic semiconductors (OSs) are based on earth abundant elements, have a tunable optoelectronic properties, and achieved an excellent solar to electricity conversion efficiency. Therefore, a rapidly growing interest has been attracted to employ OSs in PEC water splitting in recent years.[2] Until now, most of the research attention is focused on the development of OS based photocathodes, while the development of OS photoanodes[3] is lacking despite their necessity in PEC tandem devices.

Covalent polymer networks (CPNs) offer a superior robustness among various types of OSs, thus providing a route to satisfy the harsh operation requirements of photoanodes. However, the application of CPNs in optoelectronic devices is severely limited by their poor solubility and processability. Here, an in-situ CPN film preparation approach (based on thermal azide alkyne cycloaddition solid state reaction) is reported to overcome the challenge of CPN film fabrication.[4] The optoelectronic properties of the CPN films are investigated in photovoltaic devices. As a proof of concept for the application in PEC water splitting, n-type CPN semiconducting films with remarkable robustness are used for photoactive materials in photoanodes for oxygen evolution reaction (OER). After optimizing the interfacial layers and OER catalyst, a water oxidation photocurrent with the stability among the best of OS photoanodes is achieved. An outlook on the application of these CPN films toward practical solar fuel generation is finally given.

The authors thank the Swiss Competence Centre for Energy Research (SCCER Heat and Electricity Storage, contract #CTI 1155002545) and the European Research Commission (ERC starting grant “CEMOS” Project 336506) for financial support.

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