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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes
Published on: April 10, 2015
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First Study on Phosphonite-Coordinated Ruthenium Sensitizers for Efficient Photocatalytic Hydrogen Evolution
T Swetha1,2, Indranil Mondal2,3, K Bhanuprakash1,2
1Inorganic and Physical Chemistry Division, CSIR-Indian Institute of Chemical Technology , Uppal road, Tarnaka, Hyderabad-500007, India.
ACS Applied Materials & Interfaces
|August 18, 2015
Summary
New ruthenium(II) sensitizers with phosphonite ligands show high efficiency for photocatalytic hydrogen production. The GS12 complex achieved a turnover number of 8605, significantly outperforming the N719 reference.
Area of Science:
- Materials Science
- Photochemistry
- Catalysis
Background:
- Ruthenium(II) complexes are widely studied as photosensitizers.
- Efficient photocatalytic hydrogen production is crucial for renewable energy.
- Developing novel sensitizers with improved performance is an ongoing research area.
Purpose of the Study:
- To design and synthesize novel phosphonite-coordinated ruthenium(II) sensitizers.
- To evaluate their application in photocatalytic hydrogen production over a Pt-TiO2 system.
- To investigate the effect of ligand structure and pH on hydrogen evolution.
Main Methods:
- Synthesis of heteroleptic ruthenium(II) complexes (GS11, GS12, GS13) with phosphonite and ĈN̂N/terpyridine ligands.
- Characterization using UV-Vis spectroscopy and Density Functional Theory (DFT) calculations.
- Photocatalytic hydrogen evolution experiments over Pt-TiO2, measuring turnover number (TON) and pH dependence.
Main Results:
- The synthesized complexes exhibit broad metal-to-ligand charge transfer (MLCT) bands extending to 900 nm.
- DFT calculations indicate HOMO localization on Ru/Cl and LUMO on the polypyridyl ligand.
- GS12 demonstrated a maximum TON of 8605, significantly higher than the reference N719 (TON 163).
- Optimal hydrogen production yield was observed at pH 7 for all tested sensitizers.
Conclusions:
- The novel phosphonite-coordinated ruthenium(II) sensitizers are effective for photocatalytic hydrogen production.
- GS12 shows superior performance compared to existing sensitizers.
- pH 7 is optimal for hydrogen evolution using these sensitizer systems.
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