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Herein, we extend our “combined electrochemical–frustrated Lewis pair” approach to include Pt electrode surfaces for the first time. We found that the voltammetric response of an electrochemical–frustrated Lewis pair (FLP) system involving the B(C6F5)3/[HB(C6F5)3]− redox couple exhibits a strong surface electrocatalytic effect at Pt electrodes. Using a combination of kinetic competition studies in the presence of a H atom scavenger, 6-bromohexene, and by changing the steric bulk of the Lewis acid borane catalyst from B(C6F5)3 to B(C6Cl5)3, the mechanism of electrochemical–FLP reactions on Pt surfaces was shown to be dominated by hydrogen-atom transfer (HAT) between Pt, [Pt[BOND]H] adatoms and transient [HB(C6F5)3]⋅ electrooxidation intermediates. These findings provide further insight into this new area of combining electrochemical and FLP reactions, and proffers additional avenues for exploration beyond energy generation, such as in electrosynthesis.
|Number of pages||7|
|Journal||Chemistry - A European Journal|
|Early online date||6 Nov 2014|
|Publication status||Published - 7 Jan 2015|
- cyclic voltammetry
- frustrated Lewis pairs
- fuel cells
- hydrogen transfer
- 1 Finished
(PiHOMER) Pioneering Heterogeneous Organometallic-Mediated Electrocatalytic Reactions
Wildgoose, G. & Blagg, R.
1/08/12 → 31/07/17
- 13 Citations (Scopus)
- 5 Article
Facile Protocol for Water-Tolerant “Frustrated Lewis Pair”-Catalyzed HydrogenationScott, D. J., Simmons, T. R., Lawrence, E. J., Wildgoose, G. G., Fuchter, M. J. & Ashley, A. E., 17 Aug 2015, In: ACS Catalysis. 5, 9, p. 5540-5544
Research output: Contribution to journal › Article › peer-reviewOpen AccessFile88 Citations (Scopus)20 Downloads (Pure)
An Electrochemical Study of Frustrated Lewis Pairs: A Metal-free Route to Hydrogen OxidationLawrence, E., Oganesyan, V., Hughes, D., Ashley, A. & Wildgoose, G., 2 Apr 2014, In: Journal of the American Chemical Society. 136, 16, p. 6031-6036 6 p.
Research output: Contribution to journal › Article › peer-reviewFile43 Citations (Scopus)11 Downloads (Pure)
Metal-Free Dihydrogen Oxidation by a Borenium Cation: A Combined Electrochemical/Frustrated Lewis Pair ApproachLawrence, E. J., Herrington, T. J., Ashley, A. E. & Wildgoose, G. G., 8 Sep 2014, In: Angewandte Chemie International Edition. 53, 37, p. 9922–9925 4 p.
Research output: Contribution to journal › Article › peer-reviewFile23 Citations (Scopus)8 Downloads (Pure)
Best Young Energy Storage Scientist Award 2015
Wildgoose, G. (Recipient), 2015
Prize: Prize (including medals and awards)