Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 21, Pages 6229-6234Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201601653
Keywords
amphiphilic complexes; catalysis; ruthenium complex; self-assembly; water oxidation
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Funding
- Ministry of Science and Technology of China [2013CB834505, 2014CB239402, 2013CB834804]
- National Natural Science Foundation of China [91427303, 21390404, 51373193]
- Chinese Academy of Sciences [KGZD-EW-T05]
- Chinese Academy of Sciences
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The oxidation of water to molecular oxygen is the key step to realize water splitting from both biological and chemical perspective. In an effort to understand how water oxidation occurs on a molecular level, a large number of molecular catalysts have been synthesized to find an easy access to higher oxidation states as well as their capacity to make O-O bond. However, most of them function inamixture of organic solvent and water and the O-O bond formation pathway is still a subject of intense debate. Herein, we design the first amphiphilic Ru-bda (H(2)bda= 2,2'-bipyridine-6,6'-dicarboxylic acid) water oxidation catalysts (WOCs) of formula [Ru-II(bda)(4-OTEG-pyridine)(2)] (1, OTEG = OCH2CH2OCH2CH2OCH3) and [Ru-II(bda)(PySO3Na)(2)] (2, PySO3- = pyridine-3-sulfonate), which possess good solubility in water. Dynamic light scattering (DLS), scanning electron microscope (SEM), critical aggregation concentration (CAC) experiments and product analysis demonstrate that they enable to self-assemble in water and form the O-O bond through different routes even though they have the same bda(2-) backbone. This work illustrates for the first time that the O-O bond formation pathway can be regulated by the interaction of ancillary ligands at supramolecular level.
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