Abstract
Ru-Based complexes have advanced the study of molecular water oxidation catalysts (WOCs) both in catalysis and mechanism. The electronic effect has always been considered as an essential factor for the catalyst properties while less attention has been focused on the bite angle effect on water oxidation catalysis. The Ru-bda ([Ru(bda)(pic)2]; bda2- = 2,2'-bipyridine-6,6'-dicarboxylate; pic = 4-picoline) catalyst is one of the most active WOCs and it has a largely distorted octahedral configuration with an O-Ru-O bite angle of 123°. Herein, we replaced the carboxylate (-COO-) groups of bda2- with two methylenesulfonate (-CH2SO3-) groups and prepared a negatively charged ligand, bms2- (2,2'-bipyridine-6,6'-dimethanesulfonate), and the Ru-bms complex [Ru(bms)(pic)2]. The O-Ru-O bite angle changed from 123° in Ru-bda to 84° in Ru-bms, leading to a dramatic influence on the catalytic behavior. Systematic analysis of the reaction intermediates suggested that Ru-bms transformed all the way to Ru-bdavia oxidative decomposition under CeIV-driven water oxidation conditions.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
