Work

Dispersion forces drive water oxidation in molecular ruthenium catalysts

Year: 2020

Type: article

Abstract: calculations, we show that the thermodynamic driving force for the catalysis is obtained by modulation of π-stacking dispersion interactions within the catalytically active dimer core, supporting recently suggested mechanistic principles of Ru-based water-splitting catalysts. The dioxygen bond forms in a semi-concerted radical coupling mechanism, similar to the suggested water-splitting mechanism in photosystem II. By rationally tuning the dispersion effects, we design a new catalyst with a low activation barrier for the water-splitting. The catalytic principles are probed by synthesis, structural, and electrochemical characterization of the new catalyst, supporting enhanced water-splitting activity under the examined conditions. Our combined findings show that modulation of dispersive interactions provides a rational catalyst design principle for controlling challenging chemistries.

Source: RSC Advances

DOI: 10.1039/d0ra09004b

Authors: Mikael P. Johansson, Lukas Niederegger, Markus Rauhalahti, Corinna R. Hess, Ville R. I. Kaila

Institutions: University of Helsinki, Technical University of Munich, Stockholm University

Language: English

Topic: Electrocatalysts for Energy Conversion

Subfield: Renewable Energy, Sustainability and the Environment

Field: Energy

Domain: Physical Sciences

Open Access status: gold

Estimated APC paid: $875

Funders: Academy of Finland, Jane ja Aatos Erkon Säätiö, China Scholarship Council