Cobalt-based molecular electrocatalysis of nitrile reduction: evolving sustainability beyond hydrogen

Simon Child; Radoslav Raychev; Nathan Moss; Benjamin  Howchen; Peter N. Horton; Christopher Prior; Vasily Oganesyan; John Fielden

doi:10.1039/c9dt00773c

Cobalt-based molecular electrocatalysis of nitrile reduction: evolving sustainability beyond hydrogen

Simon Child, Radoslav Raychev, Nathan Moss, Benjamin Howchen, Peter N. Horton, Christopher Prior, Vasily Oganesyan, John Fielden

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Abstract

Two new cobalt bis-iminopyridines, [Co(DDP)(H2O)2](NO3)2 (1, DDP = cis-[1,3-bis(2-pyridinylenamine)] cyclohexane) and [Co(cis-DDOP)(NO3)](NO3) (2, cis-DDOP = cis-3,5-bis[(2- Pyridinyleneamin]-trans-hydroxycyclohexane) electrocatalyse the 4-proton, 4-electron reduction of acetonitrile to ethylamine. For 1, this reduction occurs in preference to reduction of protons to H2. A coordinating hydroxyl proton relay in 2 reduces the yield of ethylamine and biases the catalytic system back towards H2.

Original language	English
Pages (from-to)	9576-9580
Journal	Dalton Transactions
Volume	48
Issue number	26
Early online date	11 Jun 2019
DOIs	https://doi.org/10.1039/c9dt00773c
Publication status	Published - 14 Jul 2019

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10.1039/c9dt00773cLicence: CC BY

Published_VersionFinal published version, 559 KBLicence: CC BY

Vasily Oganesyan
- V.Oganesyanuea.acuk
- School of Chemistry, Pharmacy and Pharmacology - Reader in Computational Chemistry
- Centre for Molecular and Structural Biochemistry - Member
- Centre for Photonics and Quantum Science - Member
- Chemistry of Life Processes - Member
- Chemistry of Light and Energy - Member
Person: Research Group Member, Research Centre Member, Academic, Teaching & Research

Cite this

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title = "Cobalt-based molecular electrocatalysis of nitrile reduction: evolving sustainability beyond hydrogen",

abstract = "Two new cobalt bis-iminopyridines, [Co(DDP)(H2O)2](NO3)2 (1, DDP = cis-[1,3-bis(2-pyridinylenamine)] cyclohexane) and [Co(cis-DDOP)(NO3)](NO3) (2, cis-DDOP = cis-3,5-bis[(2- Pyridinyleneamin]-trans-hydroxycyclohexane) electrocatalyse the 4-proton, 4-electron reduction of acetonitrile to ethylamine. For 1, this reduction occurs in preference to reduction of protons to H2. A coordinating hydroxyl proton relay in 2 reduces the yield of ethylamine and biases the catalytic system back towards H2.",

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T1 - Cobalt-based molecular electrocatalysis of nitrile reduction: evolving sustainability beyond hydrogen

AU - Child, Simon

AU - Raychev, Radoslav

AU - Moss, Nathan

AU - Howchen, Benjamin

AU - Horton, Peter N.

AU - Prior, Christopher

AU - Oganesyan, Vasily

AU - Fielden, John

PY - 2019/7/14

Y1 - 2019/7/14

N2 - Two new cobalt bis-iminopyridines, [Co(DDP)(H2O)2](NO3)2 (1, DDP = cis-[1,3-bis(2-pyridinylenamine)] cyclohexane) and [Co(cis-DDOP)(NO3)](NO3) (2, cis-DDOP = cis-3,5-bis[(2- Pyridinyleneamin]-trans-hydroxycyclohexane) electrocatalyse the 4-proton, 4-electron reduction of acetonitrile to ethylamine. For 1, this reduction occurs in preference to reduction of protons to H2. A coordinating hydroxyl proton relay in 2 reduces the yield of ethylamine and biases the catalytic system back towards H2.

AB - Two new cobalt bis-iminopyridines, [Co(DDP)(H2O)2](NO3)2 (1, DDP = cis-[1,3-bis(2-pyridinylenamine)] cyclohexane) and [Co(cis-DDOP)(NO3)](NO3) (2, cis-DDOP = cis-3,5-bis[(2- Pyridinyleneamin]-trans-hydroxycyclohexane) electrocatalyse the 4-proton, 4-electron reduction of acetonitrile to ethylamine. For 1, this reduction occurs in preference to reduction of protons to H2. A coordinating hydroxyl proton relay in 2 reduces the yield of ethylamine and biases the catalytic system back towards H2.

U2 - 10.1039/c9dt00773c

DO - 10.1039/c9dt00773c

M3 - Article

VL - 48

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EP - 9580

JO - Dalton Transactions

JF - Dalton Transactions

SN - 1477-9226

IS - 26

ER -

Cobalt-based molecular electrocatalysis of nitrile reduction: evolving sustainability beyond hydrogen

Abstract

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