Catalysis
Ru dimer vs monomer splits CO from formate
Open access · cc by · source: Europe PMC
Dilute, bright photolysis of Ru(bpy)(CO)2Cl2 gives CO; concentrated or dim light favours a Ru(I) dimer that makes formate.
Study at a glance
- Design
- Other — Photochemical CO2 reduction with [Ru(bpy)3]2+/Ru carbonyl catalysts varying concentration and light
- N
- Molecular photocatalysis concentration-dependence study — no sample N
- Population
- DMA/water photoreduction mixtures with Ru catalysts and BNAH
- Outcome
- TON and CO/formate selectivity as a function of catalyst concentration
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Key findings
TON ~300 at 0.10 mM vs ~4000 at 5.0 μM. CO/HCOO– ~2 vs ~7 after 30 min. CO rate peaks at 20–30 μM then falls while formate keeps rising. Low light grows the 700–800 nm polymer and favours formate. The 6Mes complex gives CO only (formate = photosensitizer blank).
Methodology
Authors irradiated DMA/water (9:1) with [Ru(bpy)3]2+/BNAH, varied catalyst loading and light intensity, compared the isolated Cl-bridged dimer, and made a 6Mes-bpy analogue that cannot dimerise.
Limitations
The dimer was not detected in situ by UV-vis or ESI-MS during catalysis; how the Ru(I) dimer makes formate remains computationally open; [Ru(bpy)3]2+ itself produces blank CO/formate.
How this study connects
Role on claims
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Evidence for the claim as stated.
Dilute, bright photolysis of Ru(bpy)(CO)2Cl2 gives CO; concentrated or dim light favours a Ru(I) dimer that makes formate.
Evidence for the claim as stated.
Heterogeneous, molecular and dual photoredox/metal systems are not interchangeable; support, ligand and light each change the active site.
Evidence for the claim as stated.
Open questions
Tensions this paper is part of
From concept pages' “where studies disagree.” Disagreement means the same question; scope means different assays, populations, or outcomes.
Heterogeneous, molecular and dual photoredox/metal systems are not interchangeable; support, ligand and light each change the active site.
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