화학공학소재연구정보센터
Journal of Catalysis, Vol.369, 10-20, 2019
Rapid identification of homogeneous O-2 evolution catalysts and comparative studies of Ru(II)-carboxamides vs. Ru(II)-carboxylates in water-oxidation
One of the major challenges in developing sustainable energy storage systems is to discover robust oxygen evolving catalysts (OECs) that can efficiently oxidize water and produce oxygen, electrons and protons under highly oxidizing conditions. Thus, developing new screening methodologies and practical tools for OEC discovery is essential. Herein, we report a screening protocol which allows the accurate identification, benchmarking and kinetic analysis of molecular OECs using chemical oxidants, based on an oxygen-sensitive luminescent dissolved oxygen optical probe (DOOP). To demonstrate the practicality of this protocol, we screened more than 100 reactions to benchmark and evaluate the structure-activity relationship of several transition-metal complexes 1-16 based on Ru, Fe and Cu. Water-oxidation by Ru (II)-carboxylates is compared to structurally similar and less studied Ru(II)-carboxamides. A new Ru(II) complex 6 containing the doubly deprotonated N,N'-bis(aryl)pyridine-2,6-dicarboxamide was also synthesized and its oxygen evolution rate was found to be dramatically enhanced at neutral pH. (C) 2018 Elsevier Inc. All rights reserved.