Water oxidation electrocatalysis using ruthenium coordination oligomers adsorbed on multiwalled carbon nanotubes

• Published in: Nature chemistry 2020-11, Vol.12 (11), p.1060-1066
• Main Authors: Hoque, Md Asmaul, Gil-Sepulcre, Marcos, de Aguirre, Adiran, Elemans, Johannes A. A. W., Moonshiram, Dooshaye, Matheu, Roc, Shi, Yuanyuan, Benet-Buchholz, Jordi, Sala, Xavier, Malfois, Marc, Solano, Eduardo, Lim, Joohyun, Garzón-Manjón, Alba, Scheu, Christina, Lanza, Mario, Maseras, Feliu, Gimbert-Suriñach, Carolina, Llobet, Antoni
• Format: Article
• Language: English
• Subjects: 639/638/161; 639/638/675; 639/638/77/886; 639/638/911; Analytical Chemistry; Anchoring; Biochemistry; Catalysis; Catalysts; Chemistry; Chemistry and Materials Science; Chemistry/Food Science; Coordination; Fossil fuels; Heavy metals; Inorganic Chemistry; Multi wall carbon nanotubes; Nanotechnology; Nanotubes; Oligomers; Organic Chemistry; Oxidation; pH effects; Photoelectrochemical devices; Physical Chemistry; Ruthenium; Ruthenium compounds; Transition metals
• ISSN: 1755-4330; 1755-4349
• DOI: 10.1038/s41557-020-0548-7

Photoelectrochemical cells that utilize water as a source of electrons are one of the most attractive solutions for the replacement of fossil fuels by clean and sustainable solar fuels. To achieve this, heterogeneous water oxidation catalysis needs to be mastered and properly understood. The search continues for a catalyst that is stable at the surface of electro(photo)anodes and can efficiently perform this reaction at the desired neutral pH. Here, we show how oligomeric Ru complexes can be anchored on the surfaces of graphitic materials through CH– π interactions between the auxiliary ligands bonded to Ru and the hexagonal rings of the graphitic surfaces, providing control of their molecular coverage. These hybrid molecular materials behave as molecular electroanodes that catalyse water oxidation to dioxygen at pH 7 with high current densities. This strategy for the anchoring of molecular catalysts on graphitic surfaces can potentially be extended to other transition metals and other catalytic reactions. Efficient and stable water oxidation catalysts are important if photoelectrochemical cells are to be used to provide clean and sustainable solar fuels. A water oxidation catalyst that operates at neutral pH has now been developed that features ruthenium coordination oligomers anchored onto the surfaces of graphitic materials through CH– π interactions.