Tuning Photoredox Catalysis of Ruthenium with Palladium: Synthesis of Heterobimetallic Ru–Pd Complexes That Enable Efficient Photochemical Reduction of CO<sub>2</sub>

Yang, Siteng; Morita, Yuto; Nakamura, Yuta; Iwasawa, Nobuharu; Takaya, Jun

doi:10.1021/jacs.3c14338

J. Am. Chem. Soc.

2024

DOI: 10.1021/jacs.3c14338

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Tuning Photoredox Catalysis of Ruthenium with Palladium: Synthesis of Heterobimetallic Ru–Pd Complexes That Enable Efficient Photochemical Reduction of CO₂

Siteng Yang,

Yuto Morita,

Yuta Nakamura

et al.

Abstract: New Ru−Pd heterobimetallic complexes were synthesized and structurally characterized utilizing 6,6″bis(phosphino)-2,2′:6′,2″-terpyridine as a scaffold for the metal−metal bond. The dicationic Ru−Pd complex was found to exhibit high catalytic activity as a photocatalyst for photochemical reduction of CO 2 to CO under visible light irradiation. This study established a new design of transition metal catalysts that tune photoredox catalysis with metalloligands.

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Cited by 7 publications

References 43 publications

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Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Yu,

Chen,

Lin

et al. 2024

Angewandte Chemie

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We demonstrate an electrostatic confinement‐induced charge transfer pathway in a supramolecular photocatalyst comprising of an ionic covalent organic framework (COF) and cationic metal complexes. The dynamic electrostatic interactions not only attract cations around the COF to accept photogenerated electrons, but also allows for a retention of homogeneous catalytic characters of complexes, making a subtle balance. Accordingly, the electrostatic confinement effect facilitates the forward electron transfer from a photoexcited COF to cationic Co complex, realizing a remarkable photocatalytic CO2 reduction performance. Its catalytic efficiency is far superior to the supramolecular counterparts with Van‐der‐Waals or hydrogen bonding interactions. This work presents an insight for enhancing charge transfer in supramolecular systems, and provides an effective approach for construction of highly efficient photocatalysts.

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Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Yu,

Chen,

Lin

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Yu,

Chen,

Lin

et al. 2024

Angew Chem Int Ed

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Modular Synthesis of C₂‐Symmetric Chiral TPy‐BPI Pincer Ligands and Application in Asymmetric Ni(II)‐Catalysed Friedel‐Crafts Alkylation

Cen,

Ding,

Liu

et al. 2024

Chin. J. Chem.

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Comprehensive SummaryTerpyridine ligands have been applied as a class of unique ligands due to their rich coordination chemistry in the catalysis. Herein, we developed a new class of C2‐symmetric chiral terpyridine‐pyrroloimidazolone ligands (TPy‐BPI). Their catalytic activity was evaluated in the asymmetric Friedel‐Crafts alkylation of indoles with 2,3‐dioxopyrrolidines. Excellent yields (up to 92%) and high enantioselectivities (up to 97% ee) are obtained for a wide range of substrates under mild conditions. In addition to 2,3‐dioxopyrrolidines, β,γ‐unsaturated α‐ketoesters were also compatible in the Ni(OTf)2‐TPy‐BPI ligand L1‐catalyzed reaction. Control experiments, single crystal structure of two TPy‐BPI L1‐Ni(OTf)2 complexes, and DFT calculations revealed the origins of the enantioselectivity. To the best of our knowledge, our work is the first report showing that the terpyridine framework contained only two nitrogen atoms coordinating with the metal, and the additional pyridine unit only acted as stereodirecting element, which is different from the previously reported terpyridine ligands containing all three nitrogen atoms coordinating with the metal.

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Tuning Photoredox Catalysis of Ruthenium with Palladium: Synthesis of Heterobimetallic Ru–Pd Complexes That Enable Efficient Photochemical Reduction of CO₂

Cited by 7 publications

References 43 publications

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Modular Synthesis of C₂‐Symmetric Chiral TPy‐BPI Pincer Ligands and Application in Asymmetric Ni(II)‐Catalysed Friedel‐Crafts Alkylation

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Product

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Tuning Photoredox Catalysis of Ruthenium with Palladium: Synthesis of Heterobimetallic Ru–Pd Complexes That Enable Efficient Photochemical Reduction of CO2

Cited by 7 publications

References 43 publications

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO2 Reduction

Modular Synthesis of C2‐Symmetric Chiral TPy‐BPI Pincer Ligands and Application in Asymmetric Ni(II)‐Catalysed Friedel‐Crafts Alkylation

Contact Info

Product

Resources

About

Tuning Photoredox Catalysis of Ruthenium with Palladium: Synthesis of Heterobimetallic Ru–Pd Complexes That Enable Efficient Photochemical Reduction of CO₂

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Electrostatic Confinement‐Induced Excited Charge Transfer in Ionic Covalent Organic Framework Promoting CO₂ Reduction

Modular Synthesis of C₂‐Symmetric Chiral TPy‐BPI Pincer Ligands and Application in Asymmetric Ni(II)‐Catalysed Friedel‐Crafts Alkylation