Controlled uranyl-catalysed hydrocarbon C-H bond cleavage

Purkis, J. M., Arnold, P.L., Austin, J., Botti, A., Love, J.B. and Raukauskaite, R. (2018) Controlled uranyl-catalysed hydrocarbon C-H bond cleavage. In Nuclear Decommissioning Authority Annual Seminar 2018. Nuclear Decommissioning Authority..

Abstract

The desire to better understand the chemistry involved in its safe storage has contributed to a renaissance in the field of actinide chemistry, with uranium and its compounds experiencing a myriad of exciting recent developments [1].
The irradiation of uranyl (UVIO22+) compounds with visible light to affect chemical transformations – uranyl photo-catalysis – is one such area. Shining light on solutions containing uranyl salts has been shown to result in the destruction of aqueous organic pollutants or the fluorination of inert C-H bonds [2]. Neither are easy chemical transformations to perform.
In aqueous solution, the photo-excited state of the uranyl ion can effect C-H bond cleavage by H-atom abstraction. We recently reported the first examples of hydrocarbon C-H bond cleavage via a thermal pathway [3].
Targeting the room-temperature, environmentally-benign and chemo-selective uranyl photo-catalysed hydrocarbon transformation, we show that key transformations of common contaminants into industrially useful hydrocarbons is possible, with careful ligand design. We will present ongoing efforts to design uranyl photo-catalysts to target selective and challenging chemical transformations.
References
[1] Arnold et al., Nature, 2008, 451, 315; Liddle et al., Science, 2012, 337, 717.
[2] Krishna et al., J. Phys. Chem. C., 2008, 112, 15832; West et al., Angew. Chem. Int. Ed., 2016, 55, 8923.
[3] Arnold et al., Nat. Chem., 2010, 2, 1056.
[4] Wang et al., Inorg. Chem., 1995, 54, 6034; Yong et al., Sci. China Chem., 2013, 56, 1671

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Contributors

Author: J. M. Purkis

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