Donor-Flexible Nitrogen Ligands for Efficient Iridium-Catalyzed Water Oxidation Catalysis
Miquel Navarro1,2, Mo Li3, Helge Müller-Bunz2
1Department of Chemistry & Biochemistry, University of Bern, Freiestrasse 3, 3012, Bern, Switzerland.
A novel pyridylideneamide ligand enhances iridium-catalyzed water oxidation for solar fuel production. This dynamic ligand boosts catalytic activity and stability, crucial for efficient solar fuel devices.
Area of Science:
- Inorganic Chemistry
- Catalysis
- Solar Energy Conversion
Background:
- Water oxidation is essential for solar fuel production.
- Developing efficient and stable catalysts is a key challenge.
- Iridium complexes are promising for water oxidation catalysis.
Purpose of the Study:
- To design and utilize a dynamic pyridylideneamide ligand for iridium-catalyzed water oxidation.
- To improve the activity and stability of water oxidation catalysts.
- To advance the development of efficient solar fuel devices.
Main Methods:
- Synthesis of a pyridylideneamide ligand with tunable donor properties.
- Coordination of the ligand to a Cp* iridium center.
- Electrochemical and spectroscopic characterization of the catalytic system.
- Evaluation of catalytic performance in water oxidation.
Main Results:
- The dynamic ligand exhibits both zwitterionic and diene-type resonance structures.
- The iridium complex demonstrated a nearly three-fold increase in turnover frequency compared to benchmarks.
- Exceptionally high turnover numbers were achieved, indicating catalyst robustness.
- The catalytic cycle showed minimal degradation, highlighting ligand stability.
Conclusions:
- The pyridylideneamide ligand significantly enhances iridium-based water oxidation catalysis.
- The ligand's dynamic nature contributes to high activity and stability.
- This work represents a significant step towards efficient solar fuel generation.
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