Experimental and computational study of particle formation kinetics in UF6 hydrolysis

Literature Information

Publication Date 2020-07-30
DOI 10.1039/D0RE00207K
Impact Factor 4.239
Authors

Meng-Dawn Cheng, Jason M. Richards, Michael A. Omana, Joshua A. Hubbard, Glenn A. Fugate


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Abstract

The formation and growth of UO2F2 particles by gas-phase UF6 hydrolysis remains of interest to actinide chemistry researchers. The total number concentration of the UO2F2 aerosol particles that can be produced in the reaction is regulated primarily by the availability of water molecules under our reactor conditions. An increase in water molecule concentration corresponds with a higher amount and larger size of UO2F2 aerosol particles produced. The growth rates of aerosol particles appear to approach a single number in the range of [0.05 ± 0.03–0.08 ± 0.04] (nm s−1), as the molar ratio of water to UF6 decreases below 1. The size of primary particles produced from the UF6 hydrolysis under water-deprived conditions was estimated to be 3.6 ± 0.4 nm. As the molar ratio became greater than 1.7, the size of primary particles increased with increased availability of water molecules. The primary particle model developed in this work predicted a size range for the UO2F2 primary particles similar to that estimated based on the data from gas-phase UF6 hydrolysis experiments. This result suggests that the volume-driven coalescence process assumption used in the derivation of the primary particle model was reasonable. The ability to precisely control the availability of water molecules and reaction time could lead to the production of nearly monodispersed aerosol particles. This finding has significant implications in the engineering and manufacturing of fuel powder materials and possibly the future development and deployment of environmental sampling apparatus.

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Source Journal

Reaction Chemistry & Engineering

Reaction Chemistry & Engineering
CiteScore: 0
Self-citation Rate: 8.8%
Articles per Year: 284

Reaction Chemistry & Engineering is an interdisciplinary journal reporting cutting-edge research focused on enhancing the understanding and efficiency of reactions. Reaction engineering leverages the interface where fundamental molecular chemistry meets chemical engineering and technology. Challenges in chemistry can be overcome by the application of new technologies, while engineers may find improved solutions for process development from the latest developments in reaction chemistry. Reaction Chemistry & Engineering is a unique forum for researchers whose interests span the broad areas of chemical engineering and chemical sciences to come together in solving problems of importance to wider society. All papers should be written to be approachable by readers across the engineering and chemical sciences. Papers that consider multiple scales, from the laboratory up to and including plant scale, are particularly encouraged.

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