Carbon nitride photoanodes modified with Ru-based oligomer for enhanced activity and stability in neutral PEC for water oxidation

Martina Salati^a, Sanjit Mondal^b, Marco Nicaso^a, Carles Bo^a, Marcos Gil-Sepulcre^a^,^c, Menny Shalom^b, Antoni Llobet^a

^aInstitute of Chemical Research of Catalonia (ICIQ), Tarragona – 43007, Spain

^bBen Gurion University of the Negev (BGU), Beer Sheva - 8410501, Israel

^cMax Planck Institute for Chemical Energy Conversion (MPI), Mülheim an der Ruhr - 45470, Germany

Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)

#HOMHET - Bridging The Gap Between Homogeneous and Heterogeneous (Photo)-Electrocatalysis

Torremolinos, Spain, 2023 October 16th - 20th

Organizers: Idan Hod, Elena Mas Marzá and Menny Shalom

Poster, Martina Salati, 345
Publication date: 18th July 2023

In the last decade, carbon nitride (CN) has gained significant attention as potential metal-free light absorber in photoelectrochemical (PEC) cells. The stability, cost-effectiveness, tunable electronic characteristics and appropriate energy bands positioning make CN an excellent candidate for the anodic site of practical PECs devices, where water oxidation (WO) takes place.[1] However, CN still lacks of efficient charge separation, which can lead to high recombination rates and lower catalytic performance and stability, and its combination with a well-designed water oxidation catalyst (WOC) is pivotal to perform efficiently the WO reaction.[2] In this work, we have prepared, characterized and studied the photoelectrochemical performance of a novel hybrid assembly, formed by a thiourea-based CN (CNTM) functionalized with a Ru-based oligomeric catalyst ([Ru(tda)(4,4′-bpy)]15(4,4′-bpy), where tda2- is [2,2′:6′,2″-terpyridine]-6,6″-dicarboxylate and bpy is bipyridine), anchored through CH-π interactions on the CN surface.[3] The assembly CNTM/Ru-MC is capable to perform WO in neutral pH with a faradaic efficiency of 89% under 1 sun irradiation at atmospheric conditions, presenting also a high stability over more than 5 hours. The novel integration of molecular-based catalysts on carbon nitride photoelectrodes represents a promising way to further improve CN-based systems, besides new potential strategies to enhance the production of clear energy.

References:

[1] Volokh M.; Peng G.; Barrio J.; Shalom M. Carbon Nitride Materials for Water Splitting Photoelectrochemical Cells. Angew. Chem. Int. Ed. 2018, 58 (19), 6138-6151.

[2] Qin, J.; Barrio, J.; Peng, G.; Tzadikov, J.; Abisdris, L.; Volokh, M; Shalom, M. Direct growth of uniform carbon nitride layers with extended optical absorption towards efficient water-splitting photoanodes. Nat. Commun. 2020, 11, 4701.

[3] Hoque, A.; Gil-Sepulcre, M.; de Aguirre, A.; Elemans, J. A. A. W.; Moonshiram, D.; Matheu, R.; Shi, Y.; Benet-Buchholz, J.; Sala, X.; Malfois, M.; Solano, E.; Lim, J.; Garzón-Manjón, A.; Scheu, C.; Lanza, M.; Maseras, F.; Gimbert-Suriñach, C.; Llobet, A. Water oxidation electrocatalysis using ruthenium coordination oligomers adsorbed on multiwalled carbon nanotubes. Nat. Chem. 2020, 12 (11), 1060–1066.

Acknowledgements:

Financial support from Ministerio de Ciencia e Innovación, the European Union and Universitat Rovira i Virgili through grants PID2019-111617RB-I00 and PRE2020-093789 is gratefully acknowledged, as well as Generalitat de Catalunya and AGAUR through the reference 2021 SGR 01583.

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