The successful and well-studied water oxidation catalyst ([(terpy)(bipy)Ru(H2O)]2+) offers an exciting platform for synthetic elaboration; the extensive library of functionalized 2,2’-bipyridine and 2,2’:6’,2”-terpyridine derivatives in the coordination chemistry literature provides fertile ground for investigation of this catalyst. Recent work by Thummel’s group demonstrated that incorporation of a carboxylate pendant base into the bidentate ligand led to both enhanced turnover frequency and turnover number. Previously, our group has studied phosphonate pendant base substitution in the context of the Sun water oxidation catalyst [k2-(bis-6,6’-carboxy-2,2’-bipyridine)Ru(4-picoline)2]. We found that incorporation of a phosphonate pendant base in place of carboxylate on the bidentate ligand of the Thummel catalyst significantly enhanced performance. Synthesis, characterization, and water oxidation activity will be presented, with specific reference to catalyst durability in the presence of the chemical terminal oxidant Ce(IV).

Heteroatom pendant bases for ruthenium catalyzed water oxidation

2019 Fall National Meeting

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