Electrocatalytic water oxidation performance in an extended porous organic framework with a covalent alliance of distinct Ru sites
Bishal Boro, Mrinal Kanti Adak, Sohag Biswas, Chitra Sarkar, Yogendra Nailwal, Abhijit Shrotri, Biswarup Chakraborty, Bryan M. Wong, John Mondal
Abstract
. The robust, albeit highly conjugated, POP framework not only triggered facile electro-kinetics but also suppressed aggregation and metallic corrosion during electrolysis. In particular, the benefits of covalent integration of distinct Ru sites into the framework can modulate intermediate adsorption and charge density, which contributes to its exceptional OER activity. All of the critical steps involved in OER are complemented by Density Functional Theory (DFT) calculations, which suggest that electrocatalytic water oxidation proceeds from a closed-shell configuration to open-shell electronic configurations with high-spin states. These open-shell configurations are more stable than their closed-shell counterparts by 1 eV, improving the overall catalytic activity.