NDLI: Enhancing H<sub>2</sub> evolution performance of an immobilised cobalt catalyst by rational ligand design

Content Provider	Royal Society of Chemistry (RSC)
Author	Muresan, Nicoleta M. Reisner, Erwin Willkomm, Janina
Copyright Year	2015
Abstract	The catalyst [CoIIIBr((DO)(DOH)(4-BnPO3H2)(2-CH2py)pn)]Br, CoP3, has been synthesised to improve the stability and activity of cobalt catalysts immobilised on metal oxide surfaces. The CoP3 catalyst contains an equatorial diimine–dioxime ligand, (DOH)2pn = N2,N2′-propanediyl-bis(2,3-butanedione-2-imine-3-oxime), with a benzylphosphonic acid (4-BnPO3H2) group and a methylpyridine (2-CH2py) ligand covalently linked to the bridgehead of the pseudo-macrocyclic diimine–dioxime ligand. The phosphonic acid functionality provides a robust anchoring group for immobilisation on metal oxides, whereas the pyridine is coordinated to the Co ion to enhance the catalytic activity of the catalyst. Electrochemical investigations in solution confirm that CoP3 shows electrocatalytic activity for the reduction of aqueous protons between pH 3 and 7. The metal oxide anchor provides the catalyst with a high affinity for mesostructured Sn-doped In2O3 electrodes (mesoITO; loading of approximately 22 nmol cm−2) and the electrostability of the attached CoP3 was confirmed by cyclic voltammetry. Finally, immobilisation of the catalyst on ruthenium-dye sensitised TiO2 nanoparticles in aqueous solutions in the presence of a hole scavenger establishes the activity of the catalyst in this photocatalytic scheme. The advantages of the elaborate catalyst design in CoP3 in terms of stability and catalytic activity are shown by direct comparison with previously reported phosphonated Co catalysts. We therefore demonstrate that rational ligand design is a viable route for improving the performance of immobilised molecular catalysts.
Starting Page	2727
Ending Page	2736
Page Count	10
File Format	HTM / HTML PDF
ISSN	20416520
Volume Number	6
Issue Number	5
Journal	Chemical Science
DOI	10.1039/c4sc03946g
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Subscribed
Subject Keyword	Health department Cyclic voltammetry Provincial Highway 3 (Taiwan) Picoline Pyridine Ligand Carboxylic acid Oxime Ion Scavenger Imine Cobalt
Content Type	Text
Resource Type	Article
Subject	Chemistry

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