Abstract
We report on the synchrotron hard X-ray-induced decomposition of strontium oxalate (SrC2O4) pressurized to 7 GPa inside a diamond anvil cell (DAC). After some 4 h of irradiation in a white X-ray synchrotron beam, a dark reddish/brown region formed in the area of irradiation which was surrounded by a yellowish brown remainder in the rest of the sample. Upon depressurization of the sample to ambient conditions, the reacted/decomposed sample was recoverable as a dark brown/red and yellow waxy solid. Synchrotron infrared spectroscopy confirmed the strong presence of CO2 even under ambient conditions with the sample exposed to air and other strongly absorbing regions, suggesting that the sample may likely be polymerized CO (in part) with dispersed CO2 and SrO trapped within the polymer. These results will have significant implications in the ability to readily produce and trap CO2 in situ via irradiation of a simple powder for useful hard X-ray photochemistry and in the ability to easily manufacture polymeric CO (via loading of powders in a DAC or high volume press) without the need for the dangerous and complex loading of toxic CO. A novel means of X-ray-induced polymerization under extreme conditions has also been demonstrated.
Highlights
Our recent efforts to develop useful hard X-ray photochemistry
It is immediately evident that a very dark cross pattern has been formed after irradiation which was in the shadow of the incident X-ray beam
We have observed that hard X-ray irradiation of strontium oxalate has initiated a powerful chemical reaction(s) which polymerized the sample and produced CO2 and SrO in situ within the poly-carbon monoxide (CO) matrix
Summary
Michael Pravica’s research group studies matter subjected to extreme conditions of pressure, temperature, and ionizing radiation They have been developing the field of useful hard X-ray photochemistry by harnessing the highly ionizing, highly penetrating, and highly focused properties of synchrotron hard X-rays (>7 keV) to initiate novel in situ decomposition and synthetic chemistry under extreme and/or isolated conditions. We have discovered an alternative and novel route of synthesis of polymeric carbon monoxide (CO) using strontium oxalate as the starting material via a combination of X-rayirradiation and high pressure without the need to use toxic CO as the reactant This is the first reported polymerization of any compound using a combination of highpressure and hard X-ray irradiation to the best of our knowledge. We seek to produce detonation products (CO2, H2O, N2, N2O, etc.) in a highly controllable way utilizing useful hard X-ray photochemistry as a means to examine the effect of mixing (Pravica, Sneed, White, et al, 2014b; Pravica et al, 2015) on intermolecular potentials via Raman and infrared (IR) spectroscopy to aid in developing better codes to predict detonation behavior of explosives (https://www-pls.llnl. gov/?url=science_and_technology-chemistry-cheetah)
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