Jump to main content
Jump to site search

Issue 12, 2014
Previous Article Next Article

Development and understanding of cobaloxime activity through electrochemical molecular catalyst screening

Author affiliations

Abstract

Electrochemical molecular catalyst screening (EMoCS) has been developed. This technique allows fast analysis and identification of homogeneous catalytic species through tandem catalyst assembly and electrochemistry. EMoCS has been used to study molecular proton reduction catalysts made from earth abundant materials to improve their viability for water splitting systems. The efficacy of EMoCS is proven through investigation of cobaloxime proton reduction activity with respect to the axial ligand in aqueous solution. Over 20 axial ligands were analysed, allowing rapid identification of the most active catalysts. Structure–activity relationships showed that more electron donating pyridine ligands result in enhanced catalytic currents due to the formation of a more basic Co–H species. The EMoCS results were validated by isolating and assaying the most electroactive cobaloximes identified during screening. The most active catalyst, [CoIIICl(dimethyl glyoximato)2(4-methoxypyridine)], showed high electro- and photoactivity in both anaerobic and aerobic conditions in pH neutral aqueous solution.

Graphical abstract: Development and understanding of cobaloxime activity through electrochemical molecular catalyst screening

Back to tab navigation

Supplementary files

Publication details

The article was received on 06 Jan 2014, accepted on 30 Jan 2014 and first published on 06 Feb 2014


Article type: Paper
DOI: 10.1039/C4CP00453A
Citation: Phys. Chem. Chem. Phys., 2014,16, 5739-5746
  • Open access: Creative Commons BY license
  •   Request permissions

    Development and understanding of cobaloxime activity through electrochemical molecular catalyst screening

    D. W. Wakerley and E. Reisner, Phys. Chem. Chem. Phys., 2014, 16, 5739
    DOI: 10.1039/C4CP00453A

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements