Chemical method for evaluating catalytic turnover frequencies (TOF) of moderate to slow H2 oxidation electrocatalysts

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dc.contributor.author Arnab Dutta
dc.contributor.author Wendy J. Shaw
dc.date.accessioned 2019-04-11T09:19:52Z
dc.date.available 2019-04-11T09:19:52Z
dc.date.issued 2019-06
dc.identifier.citation Dutta, Arnab and Shaw, Wendy J., "Chemical method for evaluating catalytic turnover frequencies (TOF) of moderate to slow H2 oxidation electrocatalysts", Organometallics, DOI: 10.1021/acs.organomet.8b00580, vol. 38, no. 6, pp. 1311-1316, Mar. 2019. en_US
dc.identifier.issn 1520-6041
dc.identifier.issn 0276-7333
dc.identifier.uri https://doi.org/10.1021/acs.organomet.8b00580
dc.identifier.uri https://repository.iitgn.ac.in/handle/123456789/4376
dc.description.abstract Hydrogen has emerged as a long-term option for storing energy from renewable resources and has led the scientific community to develop enzyme-inspired catalysts for hydrogen oxidation and production. One of the most productive families of catalysts for H2 oxidation is the pendant amine containing bis(diphosphine)nickel catalysts. Many derivatives of these nickel complexes have been prepared with varying peripheral functionalities to understand their structure-function relationship. Electrocatalysis is currently utilized as the primary tool to measure the catalytic turnover frequencies (TOFs) of these complexes; however, it does not allow accurate determination of TOFs for slow (<1 s-1) to moderately active (<1-10 s-1) catalysts, and for the slowest catalysts, it can be difficult to determine if they are turning over at all. Further, it does not allow the determination of the TOF in bulk solution. In this work, we demonstrate that a redox chemical procedure involving a change between ferrocenium cation and ferrocene can be utilized to monitor H2 oxidation catalysts. The ferrocenium cation reoxidizes the reduced nickel catalyst stoichiometrically in the presence of H2. The change of ferrocenium cation to ferrocene can be monitored in both organic and aqueous solvents via either optical spectroscopy or NMR spectroscopy. Thus, this chemical method complements the existing electrocatalytic procedure and may help to unravel the intricate details of even the slowest H2 oxidation catalysts.
dc.description.statementofresponsibility by Dutta Arnab and Wendy J. Shaw
dc.format.extent vol. 38, no. 6, pp. 1311-1316
dc.language.iso en en_US
dc.publisher American Chemical Society en_US
dc.title Chemical method for evaluating catalytic turnover frequencies (TOF) of moderate to slow H2 oxidation electrocatalysts en_US
dc.type Article en_US
dc.relation.journal Organometallics


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