Yields of primary species in the low-linear energy transfer radiolysis of water in the temperature range of 25–700 °C

Literature Information

Publication Date 2020-03-18
DOI 10.1039/D0CP00601G
Impact Factor 3.676
Authors

Abida Sultana, Jintana Meesungnoen, Jean-Paul Jay-Gerin


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Abstract

Monte Carlo track chemistry simulations were used to calculate the time-dependent yields (G values) for the radical (eaq−, H˙, ˙OH) and molecular (H2, H2O2) “primary species” formed in the low-linear energy transfer (LET) radiolysis of deaerated, pure water (H2O) in the range of ∼1 ps to 1 ms between 25 and 700 °C, at 25 MPa pressure. Beyond the critical point, we used in the calculations the new supercritical water (SCW) radiolysis database of Liu et al., in particular their reported reaction rate constants. A striking conclusion of these simulations is the sharp increase in G(˙OH) and G(H2), and the corresponding decrease in G(H˙), which are observed above 200 °C, due to the oxidation of water by the H˙ atom (H˙ + H2O → ˙OH + H2) in the homogeneous chemical stage of radiolysis. These results may have important implications for proposed Generation-IV SCW-cooled reactors for the control and management of water chemistry and for the maintenance of the structural integrity of materials.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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