Electrocatalytic reduction of CO2 with CCC-NHC pincer nickel complexes

James D. Cope; Nalaka P. Liyanage; Paul J. Kelley; Jason A. Denny; Edward J. Valente; Charles Edwin Webster; Jared H. Delcamp; T. Keith Hollis

doi:10.1039/C6CC06537F

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Electrocatalytic reduction of CO₂ with CCC-NHC pincer nickel complexes†

James D. Cope,

^a Nalaka P. Liyanage,

^b Paul J. Kelley,^b Jason A. Denny,

^a Edward J. Valente,^c Charles Edwin Webster,

*^a Jared H. Delcamp

*^b and T. Keith Hollis

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry and the Center for Computational Sciences, Mississippi State University, Mississippi State, MS, USA
E-mail: ewebster@chemistry.msstate.edu, khollis@chemistry.msstate.edu

^b Department of Chemistry and Biochemistry, The University of Mississippi, University, MS, USA
E-mail: delcamp@olemiss.edu

^c University of Portland Diffraction Facility, 112A Swindells Hall, Department of Chemistry, University of Portland, 5000 North Willamette Blvd, Portland, OR, USA

Abstract

A CCC-NHC pincer Ni(II)Cl complex was prepared according to the metallation/transmetallation methodology. It was fully characterized by electrochemical, NMR spectroscopic, theoretical, and X-ray crystallographic methods. The complex and its cation were evaluated for electrocatalytic reduction of CO₂ under a variety of conditions and found to provide some of the fastest catalytic rates and highest substrate selectivities (CO₂vs. H⁺) reported. Rates improved in the presence of water and, significantly, catalysis occurred at the first reduction potential, presumably at the Ni(I) state. Controlled potential electrolysis (CPE) was found to yield CO at 34% and formate at 47% Faradaic efficiency (FE).

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Article information

DOI: https://doi.org/10.1039/C6CC06537F
Article type: Communication
Submitted: 09 Aug 2016
Accepted: 09 Jun 2017
First published: 09 Aug 2017

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Chem. Commun., 2017,53, 9442-9445

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Electrocatalytic reduction of CO₂ with CCC-NHC pincer nickel complexes

J. D. Cope, N. P. Liyanage, P. J. Kelley, J. A. Denny, E. J. Valente, C. E. Webster, J. H. Delcamp and T. K. Hollis, Chem. Commun., 2017, 53, 9442 DOI: 10.1039/C6CC06537F

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Chemical Communications