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- Title
Improvement of Electrochemical Water Oxidation by Fine-Tuning the Structure of Tetradentate N<sub>4</sub> Ligands of Molecular Copper Catalysts.
- Authors
ShEN, Junyu; Wang, Mei; Gao, Jinsuo; Han, Hongxian; Liu, Hong; Sun, LichENg
- Abstract
Two copper complexes, [( L1)Cu(OH2)](BF4)2 [ 1; L1= N, N′-dimethyl- N, N′-bis(pyridin-2-ylmethyl)-1,2-diaminoethane] and [( L2)Cu(OH2)](BF4)2 [ 2, L2=2,7-bis(2-pyridyl)-3,6-diaza-2,6-octadiene], were prepared as molecular water oxidation catalysts. Complex 1 displayed an overpotential ( η) of 1.07 V at 1 mA cm−2 and an observed rate constant ( kobs) of 13.5 s−1 at η 1.0 V in pH 9.0 phosphate buffer solution, whereas 2 exhibited a significantly smaller η (0.70 V) to reach 1 mA cm−2 and a higher kobs (50.4 s−1) than 1 under identical test conditions. Additionally, 2 displayed better stability than 1 in controlled potential electrolysis experiments with a faradaic efficiency of 94 % for O2 evolution at 1.58 V, when a casing tube was used for the Pt cathode. A possible mechanism for 1- and 2-catalyzed O2 evolution reactions is discussed based on the experimental evidence. These comparative results indicate that fine-tuning the structures of tetradentate N4 ligands can bring about significant change in the performance of copper complexes for electrochemical water oxidation.
- Subjects
OXIDATION; CHEMICAL reactions; CHEMICAL synthesis; ELECTROCATALYSTS; CATALYTIC activity
- Publication
ChemSusChem, 2017, Vol 10, Issue 22, p4581
- ISSN
1864-5631
- Publication type
Article
- DOI
10.1002/cssc.201701458