Photoelectrochemical Reactions with Thin films towards High Value Small Organic Molecules

Daria Corsi^a, Gabriel Chan^b, Dr. Oleksandr Savateev^c, Dr. Paolo Giusto^b, Dr. Joshua P. Barham^a

^aUniversity of Regensburg

^bDepartment of Colloid ChemistryMax Planck Institute of Colloids and Interfaces14476 Potsdam, Germany

^cThe Chinese University of Hong Kong, The Chinese University of Hong Kong, Hong Kong , 0, Hong Kong

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)

Interlinking heterogeneous catalysts, mechanisms, and reactor concepts for dinitrogen reduction - #Nitroconversion

Sevilla, Spain, 2025 March 3rd - 7th

Organizers: Roland Marschall, Jennifer Strunk and Dirk Ziegenbalg

Poster, Daria Corsi, 576
Publication date: 16th December 2024

Photoelectrochemistry (PEC) with homogeneous molecular catalysts is a well-established practice and, in the field of organic chemistry, can be applied to achieve the activation of more complex molecules.^[^1-12^] However, this practice has its limitations. In fact, homogeneous catalysts can, for example, decompose, have a limited commercial availability, are difficult to synthesize and recover, and photobleach. ^[^13-21^] These problematics led to the rise of semiconductor materials, in which the pivotal concept of molecular orbitals HOMO and LUMO of homogeneous catalysts is substituted by that of the valence band (VB) and conduction band (CB). The difference between these two energy levels is called the ‘band gap’ which, for example, can be tuned by doping the material with different elements, such as carbon, nitrogen, or even metals. ^[22^-25^]In the field of organic chemistry, interfacial photoelectrochemistry (iPEC) with semiconductors could offer benefits -including catalyst cost-efficiency, reusability and stability- and could be a step further to a more sustainable future. ^[26^-27^] Graphitic carbon nitrides (g-CNs) are promising semiconductors, as they have a straightforward synthesis and are made of non-toxic elements. ^[28-34] While the band gap of g-CN materials depends on the structure, those with the chemical composition of C₃N₄ have a band gap in the range 2.6 – 2.9 eV ^[35-38] with absorption in the visible light range, all favorable characteristics to engage difficult and unactivated organic substrate.

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Acknowledgements:

All authors thank the German Research Foundation (Deutsche Forschungsgemeinschaft) for providing financial support for this project under the Priority Programme (Schwerpunktprogramme) SPP 2370 “Nitroconversion”. P. G. and G. C. thank the Max Planck Society for ongoing financial support. O. S. thanks the Chinese University of Hong Kong for ongoing financial support and the Max Planck Society for financial support at the conception of this project. J.P.B. thanks the University of Strathclyde for ongoing financial support. J.P.B. thanks the Alexander von Humboldt Foundation for funding, provided within the framework of the Sofja Kovalevskaja Award, endowed to J.P.B. by the German Federal Ministry of Education and Research, for financial support at the conception of this project.

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