Fernando, NK;
Cairns, AB;
Murray, CA;
Thompson, AL;
Dickerson, JL;
Garman, EF;
Ahmed, N;
... Regoutz, A; + view all
(2021)
Structural and Electronic Effects of X-ray Irradiation on Prototypical [M(COD)Cl]₂ Catalysts.
The Journal of Physical Chemistry A
, 125
(34)
pp. 7473-7488.
10.1021/acs.jpca.1c05759.
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Abstract
X-ray characterization techniques are invaluable for probing material characteristics and properties, and have been instrumental in discoveries across materials research. However, there is a current lack of understanding of how X-ray-induced effects manifest in small molecular crystals. This is of particular concern as new X-ray sources with ever-increasing brilliance are developed. In this paper, systematic studies of X-ray–matter interactions are reported on two industrially important catalysts, [Ir(COD)Cl]2 and [Rh(COD)Cl]2, exposed to radiation in X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) experiments. From these complementary techniques, changes to structure, chemical environments, and electronic structure are observed as a function of X-ray exposure, allowing comparisons of stability to be made between the two catalysts. Radiation dose is estimated using recent developments to the RADDOSE-3D software for small molecules and applied to powder XRD and XPS experiments. Further insights into the electronic structure of the catalysts and changes occurring as a result of the irradiation are drawn from density functional theory (DFT). The techniques combined here offer much needed insight into the X-ray-induced effects in transition-metal catalysts and, consequently, their intrinsic stabilities. There is enormous potential to extend the application of these methods to other small molecular systems of scientific or industrial relevance.
| Type: | Article |
|---|---|
| Title: | Structural and Electronic Effects of X-ray Irradiation on Prototypical [M(COD)Cl]₂ Catalysts |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.jpca.1c05759 |
| Publisher version: | https://doi.org/10.1021/acs.jpca.1c05759 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | X-rays, Catalysts, Diffraction, Transition metals, Irradiation |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10135133 |
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