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Modifying Ru-bda Backbone with Steric Hindrance and Hydrophilicity: Influence of Secondary Coordination Environments on Water-Oxidation Mechanism.
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(English)In: Article in journal (Other academic) Submitted
Abstract [en]

Understanding the seven coordination and O−O coupling pathway of the distinguished Ru-bda catalysts is essential for the development of next generation efficient water-oxidation catalysts based on earth-abundant metals. This work reports the synthesis, characterization and catalytic properties of a monomeric ruthenium catalyst Ru-bnda (H2bnda = 2,2'-bi(nicotinic acid)-6,6'-dicarboxylic acid) featuring steric hindrance and enhanced hydrophilicity on the backbone. Combining experimental evidence with systematic density functional theory calculations on the Ru-bnda and related catalysts Ru-bda, Ru-pda and Ru-biqa, we emphasized that seven coordination clearly determines presence of RuV=O with high spin density on the ORuV=O atom, i.e. oxo with radical properties, which is one of the necessary conditions for reacting through the O−O coupling pathway. However, an additional factor to make the condition sufficient is the favorable intermolecular face-to-face interaction for the generation of the pre-reactive [RuV=O···O=RuV], which is significantly influenced by the secondary coordination environments. This work provides a new understanding of the structure-activity relationship of water-oxidation catalysts and their potential to adopt I2M pathway for O−O bond formation.

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URN: urn:nbn:se:kth:diva-250268OAI: oai:DiVA.org:kth-250268DiVA, id: diva2:1307457
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QCR 20190618

Available from: 2019-04-26 Created: 2019-04-26 Last updated: 2019-06-18Bibliographically approved

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Shaoqi, Zhan
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