Sökning: onr:"swepub:oai:DiVA.org:kth-250268" >
Modifying Ru-bda Ba...
Modifying Ru-bda Backbone with Steric Hindrance and Hydrophilicity: Influence of Secondary Coordination Environments on Water-Oxidation Mechanism.
-
Biaobiao, Zhang (författare)
-
Shaoqi, Zhan (författare)
-
Tianqi, Liu (författare)
-
visa fler...
-
Linqin, Wang (författare)
-
A. Ken, Inge (författare)
-
Lele, Duan (författare)
-
Brian J.J., Timmer (författare)
-
Oleksandr, Kravchenko (författare)
-
Fei, Li (författare)
-
Mårten S. G., Ahlquist (författare)
-
Licheng, Sun (författare)
-
visa färre...
- Engelska.
- Relaterad länk:
-
https://urn.kb.se/re...
Abstract
Ämnesord
Stäng
- 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.
Publikations- och innehållstyp
- vet (ämneskategori)
- art (ämneskategori)
Hitta via bibliotek
Till lärosätets databas
- Av författaren/redakt...
-
Biaobiao, Zhang
-
Shaoqi, Zhan
-
Tianqi, Liu
-
Linqin, Wang
-
A. Ken, Inge
-
Lele, Duan
-
visa fler...
-
Brian J.J., Timm ...
-
Oleksandr, Kravc ...
-
Fei, Li
-
Mårten S. G., Ah ...
-
Licheng, Sun
-
visa färre...
- Av lärosätet
-
Kungliga Tekniska Högskolan