Synthesis, Characterization, and Catalytic CO<sub>2</sub> Reduction Reactivity of Ruthenium CNC Pincer Complexes Containing Macrocyclic or Long Chain Wingtips

Silprakob, Weerachai; Ferdous, Jannatul; Das, Sanjit; Jurss, Jonah W.; Papish, Elizabeth T.

doi:10.1021/acs.organomet.4c00282

Organometallics

2024

DOI: 10.1021/acs.organomet.4c00282

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Synthesis, Characterization, and Catalytic CO₂ Reduction Reactivity of Ruthenium CNC Pincer Complexes Containing Macrocyclic or Long Chain Wingtips

Weerachai Silprakob,

Jannatul Ferdous,

Sanjit Das

et al.

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2024

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Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

Manafe,

Olajide,

Boudreaux

et al. 2024

Organometallics

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Nickel(II) complexes bearing tetradentate NCCN ligands composed of optionally protic pyridine and N-heterocyclic carbene (NHC) donors have been synthesized and used as catalysts for carbon dioxide reduction. These complexes were synthesized bearing OMe, OBn, or OH substituents on the pyridine rings and were characterized by 1 H NMR, 13 C NMR, UV−vis, IR, HR-MS, and single crystal X-ray diffraction. The OH substituent was partially deprotonated, as shown by the crystal structure. Electrochemical studies show that these nickel complexes undergo two electron reduction events prior to CO 2 reduction. Catalytic current enhancement under CO 2 relative to N 2 is not observed under dry conditions, but the addition of proton sources leads to modest current enhancement (i cat /i p < 2). Visible light driven photochemical CO 2 reduction with a photosensitizer (Ir(ppy) 3 , where ppy = 2-phenylpyridine) and sacrificial electron and proton donors was studied, and formate is the major product with ∼10:1 formate to CO production. Electron donor groups (OMe, OBn, OH) do not enhance formate production (relative to the unsubstituted analogue), and CO production is only slightly enhanced. Overall with Ni(II), the tetradentate ligands are comparable to recently published pincer ligands for sensitized CO 2 reduction, but pincer ligands offer a clear advantage in self-sensitized catalysis.

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Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

Manafe,

Olajide,

Boudreaux

et al. 2024

Organometallics

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show abstract

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Synthesis, Characterization, and Catalytic CO₂ Reduction Reactivity of Ruthenium CNC Pincer Complexes Containing Macrocyclic or Long Chain Wingtips

Cited by 1 publication

References 45 publications

Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

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Synthesis, Characterization, and Catalytic CO2 Reduction Reactivity of Ruthenium CNC Pincer Complexes Containing Macrocyclic or Long Chain Wingtips

Cited by 1 publication

References 45 publications

Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

Nickel(II) Complexes Bearing Electron Donating OR/OH Groups on a Tetradentate Ligand Scaffold for Photocatalytic Carbon Dioxide Reduction

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Synthesis, Characterization, and Catalytic CO₂ Reduction Reactivity of Ruthenium CNC Pincer Complexes Containing Macrocyclic or Long Chain Wingtips