Electrochemical NADH Regeneration Mediated by Pyridine Amidate Iridium Complexes Interconverting 1,4- and 1,6-NADH

Trotta, Caterina; Menendez Rodriguez, Gabriel; Zuccaccia, Cristiano; Macchioni, Alceo

doi:10.1021/acscatal.4c02548

ACS Catal.

2024

DOI: 10.1021/acscatal.4c02548

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Electrochemical NADH Regeneration Mediated by Pyridine Amidate Iridium Complexes Interconverting 1,4- and 1,6-NADH

Caterina Trotta,

Gabriel Menendez Rodriguez,

Cristiano Zuccaccia

et al.

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2024

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Cited by 4 publications

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Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Boccalon,

Menendez Rodriguez,

Trotta

et al. 2024

Eur J Inorg Chem

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Glycerol, a by‐product of biodiesel production, has gained prominence as a precious platform chemical. To enhance the economic viability of the biodiesel production process and address the surplus of glycerol production, it is essential to transform it into value‐added products. In this context, homogeneous catalysis offers a promising avenue for glycerol valorisation. In this study, we introduce a family of iridium complexes bearing picolineamidate ligands with glucose‐functionalised substituents as novel homogeneous catalysts for glycerol to hydrogen and lactic acid conversion. These complexes exhibit high activity (conversion up to 53.3%) and 99% selectivity after 24 hours of reaction (TOFMAX=159 h‐1, TON24h=2498). Notably, the reaction occurs under ambient air and at milder temperature conditions (120°C) compared to other catalysts. These efforts in glycerol valorisation contribute to reducing biodiesel production costs, increasing the competitiveness of biofuels against petroleum‐based liquid fuels, giving rise to H2, through a global process with negative carbon dioxide emission, and lactic acid utilizable, among other, as a monomer for the synthesis of biodegradable plastics.

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Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Boccalon,

Menendez Rodriguez,

Trotta

et al. 2024

Eur J Inorg Chem

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Micellar Transfer Hydrogenation Catalysis in Water with Monocarbonyl Ruthenium(II)-poly(vinylphosphonate)-Containing Polymers: Achieving Reduction of Biomass-Derived Aldehydes

Lovison,

Weingarten,

Sebeschuk

et al. 2024

ACS Appl. Polym. Mater.

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With the aim to build a supramolecular organometallic catalyst for transfer hydrogenation (TH) reactions of hydrophobic substrates, micellar architectures of different sizes were obtained using amphiphilic diblock copolymers (BCPs) tethered to a Ru(II) monocarbonyl complex. An end-group functionalization strategy was employed to incorporate a bipyridyl end-group, used to further coordinate the cationic ruthenium fragment, to amphiphilic poly(2-vinylpyridine)-b-poly(diethyl vinylphosphonate). Owing to their amphiphilic character, the polymers form spherical micelles in water, which were characterized by different spectroscopic and analytical methods at different pH values and temperatures. The most suitable core−shell micellar system could level the catalytic activity of the ruthenium complex toward hydrophobic and biomass-derived aldehydes, which could be successfully reduced to the corresponding alcohols in water using potassium formate as a hydride source. Depending on the substrate's hydrophobicity and concentration, the catalytic activity varied significantly. In addition, the polymer's properties hardly changed during catalysis, facilitating effective recycling until the third catalytic cycle.

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Reversible Electrocatalytic NAD⁺/NADH Interconversion Mediated by a Pyrazine-Amidate Iridium Complex

Rodriguez,

Trotta,

Tensi

et al. 2024

J. Am. Chem. Soc.

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Electrochemical NADH Regeneration Mediated by Pyridine Amidate Iridium Complexes Interconverting 1,4- and 1,6-NADH

Cited by 4 publications

References 84 publications

Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Micellar Transfer Hydrogenation Catalysis in Water with Monocarbonyl Ruthenium(II)-poly(vinylphosphonate)-Containing Polymers: Achieving Reduction of Biomass-Derived Aldehydes

Reversible Electrocatalytic NAD⁺/NADH Interconversion Mediated by a Pyrazine-Amidate Iridium Complex

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Electrochemical NADH Regeneration Mediated by Pyridine Amidate Iridium Complexes Interconverting 1,4- and 1,6-NADH

Cited by 4 publications

References 84 publications

Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Acceptorless Dehydrogenation of Glycerol Catalysed by Ir(III) Complexes with Carbohydrate‐Functionalised Ligands: A Sweet Pathway to Produce Hydrogen and Lactic Acid

Micellar Transfer Hydrogenation Catalysis in Water with Monocarbonyl Ruthenium(II)-poly(vinylphosphonate)-Containing Polymers: Achieving Reduction of Biomass-Derived Aldehydes

Reversible Electrocatalytic NAD+/NADH Interconversion Mediated by a Pyrazine-Amidate Iridium Complex

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Reversible Electrocatalytic NAD⁺/NADH Interconversion Mediated by a Pyrazine-Amidate Iridium Complex