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Modifying Ru-bda Ba...
Modifying Ru-bda Backbone with Steric Hindrance and Hydrophilicity: Influence of Secondary Coordination Environments on Water-Oxidation Mechanism
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Zhang, Biaobiao (författare)
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Zhan, Shaoqi (författare)
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Liu, Tianqi (författare)
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Wang, Linqin (författare)
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Inge, A. Ken (författare)
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Duan, Lele (författare)
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Timmer, Brian J.J. (författare)
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Kravchenko, Oleksandr (författare)
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Li, Fei (författare)
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Ahlquist, Mårten S. G. (författare)
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Sun, Licheng (författare)
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- Engelska.
- Relaterad länk:
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https://urn.kb.se/re...
Abstract
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- 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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Zhang, Biaobiao
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Zhan, Shaoqi
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Liu, Tianqi
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Wang, Linqin
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Inge, A. Ken
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Duan, Lele
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visa fler...
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Timmer, Brian J. ...
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Kravchenko, Olek ...
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Li, Fei
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Ahlquist, Mårten ...
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Sun, Licheng
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visa färre...
- Av lärosätet
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Kungliga Tekniska Högskolan