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Benzimidazoles as Metal-Free and Recyclable Hydrides for CO 2 Reduction to Formate

Benzimidazoles as Metal-Free and Recyclable Hydrides for CO 2 Reduction to Formate

Chern-Hooi Lim, Stefan Ilic, Abdulaziz Alherz, Brady T Worrell, Samuel S Bacon, James T Hynes, Ksenija D Glusac, Charles B Musgrave

J Am Chem Soc. 2019 Jan 9;141(1):272-280.

PMID: 30477302

Abstract:

We report a novel metal-free chemical reduction of CO2 by a recyclable benzimidazole-based organo-hydride, whose choice was guided by quantum chemical calculations. Notably, benzimidazole-based hydride donors rival the hydride-donating abilities of noble-metal-based hydrides such as [Ru(tpy)(bpy)H]+ and [Pt(depe)2H]+. Chemical CO2 reduction to the formate anion (HCOO-) was carried out in the absence of biological enzymes, a sacrificial Lewis acid, or a base to activate the substrate or reductant. 13CO2 experiments confirmed the formation of H13COO- by CO2 reduction with the formate product characterized by 1H NMR and 13C NMR spectroscopy and ESI-MS. The highest formate yield of 66% was obtained in the presence of potassium tetrafluoroborate under mild conditions. The likely role of exogenous salt additives in this reaction is to stabilize and shift the equilibrium toward the ionic products. After CO2 reduction, the benzimidazole-based hydride donor was quantitatively oxidized to its aromatic benzimidazolium cation, establishing its recyclability. In addition, we electrochemically reduced the benzimidazolium cation to its organo-hydride form in quantitative yield, demonstrating its potential for electrocatalytic CO2 reduction. These results serve as a proof of concept for the electrocatalytic reduction of CO2 by sustainable, recyclable, and metal-free organo-hydrides.

Chemicals Related in the Paper:

Catalog Number	Product Name	Structure	CAS Number	Price
AP14075537	Potassium tetrafluoroborate		14075-53-7	Price

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