Modelling spur chemistry for alkaline and acidic water at high temperatures

Modelling spur chemistry for alkaline and acidic water at high temperatures The effect of pH and associated ionic strength on the primary yields in the radiolysis of pressurised water has been assessed by diffusion-kinetic calculations for temperatures in the range 100–300°C. Account has been taken for ionic strength I up to 0.1 mol kg−1, assuming that the counter ions of H+ in acid solutions and of OH− in base solutions have unit charge. In acid solutions, the H+ ions react with e− aq. The decrease in G(e− aq) and the increase in G(H) with decreasing pH becomes substantial for [H+] ≥ 1 × 10−4 m, but the primary yields of oxidising species are almost constant. In alkaline solutions, the OH− anions affect the spur chemistry of radiation-generated protons and hydroxyl radicals for [OH−] ≥ 1 × 10−4 m. The scavenging of H atoms and hydrogen peroxide becomes significant for [OH−] ≥ 1 × 10−2 m. The total yields G(OH) + G(O−) and G(H2O2) + G(HO2 −) are independent of base concentration below 0.01 m. In more alkaline solutions, G(OH) + G(O−) increases, whereas G(H2O2) + G(HO2 −) decreases with increasing [OH−]. Calculations showed the substantial yield of the reaction O− + e− aq in 0.1 m base solution. Spur chemistry in alkaline hydrogenated water is not affected by the presence of H2 if less than 0.001 m of hydrogen is added. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Research on Chemical Intermediates Springer Journals

Modelling spur chemistry for alkaline and acidic water at high temperatures

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Publisher
Springer Journals
Copyright
Copyright © 2009 by Springer Science+Business Media BV
Subject
Chemistry; Inorganic Chemistry ; Physical Chemistry ; Catalysis
ISSN
0922-6168
eISSN
1568-5675
D.O.I.
10.1007/s11164-009-0053-5
Publisher site
See Article on Publisher Site

Abstract

The effect of pH and associated ionic strength on the primary yields in the radiolysis of pressurised water has been assessed by diffusion-kinetic calculations for temperatures in the range 100–300°C. Account has been taken for ionic strength I up to 0.1 mol kg−1, assuming that the counter ions of H+ in acid solutions and of OH− in base solutions have unit charge. In acid solutions, the H+ ions react with e− aq. The decrease in G(e− aq) and the increase in G(H) with decreasing pH becomes substantial for [H+] ≥ 1 × 10−4 m, but the primary yields of oxidising species are almost constant. In alkaline solutions, the OH− anions affect the spur chemistry of radiation-generated protons and hydroxyl radicals for [OH−] ≥ 1 × 10−4 m. The scavenging of H atoms and hydrogen peroxide becomes significant for [OH−] ≥ 1 × 10−2 m. The total yields G(OH) + G(O−) and G(H2O2) + G(HO2 −) are independent of base concentration below 0.01 m. In more alkaline solutions, G(OH) + G(O−) increases, whereas G(H2O2) + G(HO2 −) decreases with increasing [OH−]. Calculations showed the substantial yield of the reaction O− + e− aq in 0.1 m base solution. Spur chemistry in alkaline hydrogenated water is not affected by the presence of H2 if less than 0.001 m of hydrogen is added.

Journal

Research on Chemical IntermediatesSpringer Journals

Published: Jun 9, 2009

References

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