Synergistic Water Oxidation with Low-Energy Light via Ru(bda)(pic)2 and a Tetranuclear Ruthenium Dendrimer
Source abstract
Abstract
The synergistic combination of the ruthenium-based tetranuclear dendrimer photosensitizer with the highly efficient water oxidation catalyst Ru(bda)(pic)2 enables effective water oxidation under low-energy light irradiation in phosphate buffer 20 mM/acetonitrile 3% (pH 7). This study demonstrates that the integrated system can produce a significant amount of oxygen using visible light at wavelengths greater than 650 nm (up to 160 nmol), achieving quite good turnover number (3.5 × 10−3), high quantum yields (0.23) and enhanced stability. These results highlight the potential of this approach to efficiently drive solar water splitting for fuel production, even with low-energy illumination, thereby advancing the development of sustainable photochemical systems for solar energy conversion.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Electrocatalysts for Energy Conversion · Advanced Photocatalysis Techniques · Covalent Organic Framework Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Dipartimento di Scienze Chimiche, Biologiche, Farmaceutiche ed Ambientali, Interuniversitary Research Center for Artificial Photosynthesis (SOLAR-CHEM), Università di Messina, Viale F. Stagno d’Alcontres 31, 98166 Messina, Italy
Consiglio Nazionale delle Ricerche-Istituto per la Microelettronica e Microsistemi (CNR-IMM), Viale F. Stagno d’Alcontres 31, 98158 Messina, Italy
Dipartimento di Chimica, Biologia e Biotecnologie, Università degli Studi di Perugia, 06123 Perugia, Italy, Via dell’Elce di Sotto, 8, 06123 Perugia, Italy
Funding
University of Messina · European Union
References (38)
Show source-provided references
1. Supramolecular Assembly of Multicomponent Photoactive Systems via Cooperatively Coupled Equilibria10.1021/ja410114d ↗
2. Self-Assembly Strategies for Integrating Light Harvesting and Charge Separation in Artificial Photosynthetic Systems10.1021/ar9001735 ↗
3. The role of hydrogen bonding in excited state intramolecular charge transfer10.1039/c2cp23879a ↗
4. Catalytic oxidation of water by an oxo-bridged ruthenium dimer10.1021/ja00378a053 ↗
5. Photo-induced Electron and energy transfer in non-covalently bonded supramolecular assemblies10.1039/cs9972600365 ↗
6. Synthesis and Study of Mononuclear Ruthenium(II) Complexes of Sterically Hindering Diimine Chelates. Implications for the Catalytic Oxidation of Water to Molecular Oxygen10.1021/ic00222a008 ↗
7. A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II10.1038/nchem.1301 ↗
8. Isolated Seven-Coordinate Ru(IV) Dimer Complex with [HOHOH]− Bridging Ligand as an Intermediate for Catalytic Water Oxidation10.1021/ja9034686 ↗
9. Highly Efficient Bioinspired Molecular Ru Water Oxidation Catalysts with Negatively Charged Backbone Ligands10.1021/acs.accounts.5b00149 ↗
10. Toward Controlling Water Oxidation Catalysis: Tunable Activity of Ruthenium Complexes with Axial Imidazole/DMSO Ligands10.1021/ja309805m ↗
11. N-Thiocarbazole-based gold nanoparticles: Synthesis, characterization and anti-proliferative activity evaluation
12. Visible light-driven water oxidation by a molecular ruthenium catalyst in homogeneous system10.1021/ic9017486 ↗
13. Visible light-driven water oxidation—From molecular catalysts to photoelectrochemical cells10.1039/c1ee01276b ↗
14. Photo-hydrogen-evolving molecular devices driving visible-light-induced water reduction into molecular hydrogen: Structure–activity relationship and reaction mechanism10.1039/c0cc04708b ↗
15. Photo-induced water oxidation with tetra-nuclear ruthenium sensitizer and catalyst: A unique 4 × 4 ruthenium interplay triggering high efficiency with low-energy visible light10.1039/c0cc00444h ↗
16. The Use of a Vanadium Species As a Catalyst in Photoinduced Water Oxidation10.1021/ja5040182 ↗
17. Synthesis of a 6-nm-Long Transition-Metal–Rare-Earth-Containing Polyoxometalate10.1021/acs.inorgchem.9b02236 ↗
18. Mechanisms of molecular water oxidation in solution and on oxide surfaces10.1039/C7CS00465F ↗
19. Molecular and Heterogeneous Water Oxidation Catalysts: Recent Progress and Joint Perspectives10.1039/D0CS00978D ↗
20. Mechanism of the Quenching of the Tris(bipyridine)ruthenium(II) Emission by Persulfate: Implications for Photoinduced Oxidation Reactions10.1021/jp407573d ↗
21. Metal-based chromophores for photochemical water oxidation
22. Ultra Stable Multinuclear Metal Complexes as Homogeneous Catalysts for Visible-Light Driven Syngas Production from Pure and Diluted CO210.1016/j.jcat.2020.03.005 ↗
23. Photo-driven water oxidation performed by supramolecular photocatalysts made of Ru(II) photosensitizers and catalysts10.1063/5.0189316 ↗
24. A Bioinspired Approach Toward Efficient Supramolecular Catalysts for CO2 Conversion
25. Architecture of Supramolecular Metal Complexes for Photocatalytic CO2 Reduction: Ruthenium–Rhenium Bi- and Tetranuclear Complexes10.1021/ic048779r ↗
26. Photo- and Redox-Active Metal Dendrimers: A Journey from Molecular Design to Applications and Self-Aggregated Systems10.1002/ejic.201800507 ↗
27. Self-Assembly of Hexameric Macrocycles from PtII /Ferrocene Dimetallic Subunits—Synthesis, Characterization, Chemical Reactivity, and Oxidation Behavior10.1002/ejic.201501050 ↗
28. Photoinduced water oxidation sensitized by a tetranuclear Ru (II) dendrimer
29. Ru-bda: Unique Molecular Water-Oxidation Catalysts with Distortion Induced Open Site and Negatively Charged Ligands10.1021/jacs.8b12862 ↗
30. Dendrimers of Nanometer Size Based on Metal Complexes: Luminescent and Redox-Active Polynuclear Metal Complexes Containing up to Twenty-Two Metal Centers10.1002/chem.19950010404 ↗
31. Water Oxidation at a Tetraruthenate Core Stabilized by Polyoxometalate Ligands: Experimental and Computational Evidence To Trace the Competent Intermediates10.1021/ja905067u ↗
32. Working the Other Way Around: Photocatalytic Water Oxidation Triggered by Reductive Quenching of the Photoexcited Chromophore10.1021/jp512541s ↗
33. Ceroni, P., Credi, A., and Venturi, M. (2010). Electrochemistry of Functional Supramolecular Systems, Wiley.10.1002/9780470583463 ↗
34. Luminescent and Redox-Active Polynuclear Transition Metal Complexes10.1021/cr941154y ↗
35. Kinetics and mechanisms of charge transfer processes in photocatalytic systems: A review10.1016/j.jphotochemrev.2012.07.002 ↗
36. Molecular Design Principles for Photoactive Transition Metal Complexes: A Guide for “Photo-Motivated” Chemists10.1021/jacs.5c02096 ↗
37. Recent Progress and Future Prospects on All-Organic Polymer Dielectrics for Energy Storage Capacitors10.1021/acs.chemrev.1c00793 ↗
38. A breath of sunshine: Oxygenic photosynthesis by functional molecular architectures10.1039/D3SC03780K ↗