Reactivity of Zn+aq in high-temperature water radiolysis

Lisouskaya, Aliaksandra; Markad, Uddhav S.; Carmichael, Ian; Bartels, David M.

doi:10.1039/d2cp02434a

Reactivity of Zn⁺_aq in high-temperature water radiolysis

Journal Article · Mon Aug 08 00:00:00 EDT 2022 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/d2cp02434a· OSTI ID:1978869

^[1]; Markad, Uddhav S. ^[2]; Carmichael, Ian ^[2]; ^[2]

University of Notre Dame, IN (United States); OSTI
University of Notre Dame, IN (United States)

For this work, reactivity of transients involving Zn⁺ in high-temperature water radiolysis has been studied in the temperature range of 25–300 °C. The reduced monovalent zinc species were generated from an electron transfer process between the hydrated electron and Zn²⁺ ions using pulse radiolysis. The Zn⁺ species can subsequently be oxidized by the radiolytically-produced oxidizing species: ˙OH, H₂O₂ and ˙H. We find that the absorption of monovalent zinc is very sensitive to the pH of the medium. An absorption maximum at 306–311 nm is most pronounced at pH 7 and the signal then decreases in acidic media where the reducing electrons are competitively captured by protons. At pH values higher than 7, hydroxo-forms of Zn²⁺ are created and the maximum of the absorption signal begins to shift to the red spectral region. We find that the optical spectrum of Zn⁺_aq cannot be fully explained in terms of a charge-transfer to solvent (CTTS) process, which was previously proposed. Reaction rates of most of the recombination reactions investigated follow the empirical Arrhenius relationship at temperatures up to 200 °C and have been determined at higher temperatures for the first time. A bimolecular disproportionation reaction of Zn⁺_aq is not observed under the conditions investigated.

View Accepted Manuscript (DOE)

Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FC02-04ER15533

OSTI ID:: 1978869

Alternate ID(s):: OSTI ID: 1881352

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 33 Vol. 24; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (43)

Theoretical insight into the coordination number of hydrated $$\mathrm{Zn}^{2+}$$ Zn 2 + from gas phase to solution Jana, Chandramohan; Ohanessian, Gilles; Clavaguéra, Carine Theoretical Chemistry Accounts, Vol. 135, Issue 5 https://doi.org/10.1007/s00214-016-1887-8	journal	May 2016
Pulse radiolysis study on redox reactions of zinc(II) Domae, M.; Chitose, N.; Zuo, Z. Radiation Physics and Chemistry, Vol. 56, Issue 3 https://doi.org/10.1016/S0969-806X(99)00291-1	journal	September 1999
Zinc treatment effects on corrosion behavior of 304 stainless steel in high temperature, hydrogenated water Ziemniak, S. E.; Hanson, M. Corrosion Science, Vol. 48, Issue 9 https://doi.org/10.1016/j.corsci.2005.10.014	journal	September 2006
Influence of Zn on oxide films on Alloy 690 in borated and lithiated high temperature water Huang, Junbo; Liu, Xiahe; Han, En-Hou Corrosion Science, Vol. 53, Issue 10 https://doi.org/10.1016/j.corsci.2011.06.001	journal	October 2011
Effect of Zn injection on established surface oxide films on 316L stainless steel in borated and lithiated high temperature water Liu, Xiahe; Wu, Xinqiang; Han, En-Hou Corrosion Science, Vol. 65 https://doi.org/10.1016/j.corsci.2012.08.022	journal	December 2012
Self-repairing oxides to protect zinc: Review, discussion and prospects Thomas, S.; Birbilis, N.; Venkatraman, M. S. Corrosion Science, Vol. 69 https://doi.org/10.1016/j.corsci.2013.01.011	journal	April 2013
Insights into the zinc effect on radio-cobalt deposition on stainless steel piping surfaces under BWR conditions from experiment guided 1st principles modelling Cantatore, Valentina; Geers, Christine; Chen, Jiaxin Journal of Nuclear Materials, Vol. 540 https://doi.org/10.1016/j.jnucmat.2020.152361	journal	November 2020
A review of corrosion product transport and radiation field buildup in boiling water reactors Lin, Chien C. Progress in Nuclear Energy, Vol. 51, Issue 2 https://doi.org/10.1016/j.pnucene.2008.05.005	journal	March 2009
Reactions of Hexa-aquo Transition Metal Ions with the Hydrated Electron up to 300 °C Kanjana, Kotchaphan; Courtin, Bruce; MacConnell, Ashley The Journal of Physical Chemistry A, Vol. 119, Issue 45 https://doi.org/10.1021/acs.jpca.5b08812	journal	October 2015
Theory and applications of charge-transfer-to-solvent spectra Blandamer, Michael J.; Fox, Malcom F. Chemical Reviews, Vol. 70, Issue 1 https://doi.org/10.1021/cr60263a002	journal	February 1970
Quantum Mechanical Continuum Solvation Models Tomasi, Jacopo; Mennucci, Benedetta; Cammi, Roberto Chemical Reviews, Vol. 105, Issue 8 https://doi.org/10.1021/cr9904009	journal	August 2005
Temperature Dependence of Equilibrium and Rate Constants of Reactions Inducing Conversion between Hydrated Electron and Atomic Hydrogen Shiraishi, Hirotsugu; Sunaryo, Geni R.; Ishigure, Kenkichi The Journal of Physical Chemistry, Vol. 98, Issue 19 https://doi.org/10.1021/j100070a037	journal	May 1994
Reduction potentials of CO2- and the alcohol radicals Schwarz, H. A.; Dodson, R. W. The Journal of Physical Chemistry, Vol. 93, Issue 1 https://doi.org/10.1021/j100338a079	journal	January 1989
Effect of ion pairing on the reactivity of solvated electrons in ethyl alcohol Hickel, B. The Journal of Physical Chemistry, Vol. 82, Issue 9 https://doi.org/10.1021/j100498a008	journal	May 1978
Pulse radiolysis studies of zinc(1+) ion reactions Rabani, Joseph; Mulac, W. A.; Matheson, Max S. The Journal of Physical Chemistry, Vol. 81, Issue 2 https://doi.org/10.1021/j100517a002	journal	January 1977
Pulse radiolytic study of nickel(1+) ion. Nickel-carbon bond formation Kelm, M.; Lilie, J.; Henglein, A. The Journal of Physical Chemistry, Vol. 78, Issue 9 https://doi.org/10.1021/j100602a007	journal	April 1974
Effect of the dielectric constant on the reactivity of the solvated electron Barat, F.; Gilles, L.; Hickel, B. The Journal of Physical Chemistry, Vol. 77, Issue 13 https://doi.org/10.1021/j100632a024	journal	June 1973
Reduction of cobalt(III) complexes by monovalent zinc, cadmium, and nickel ions in aqueous solutions Meyerstein, Dan; Mulac, W. A. The Journal of Physical Chemistry, Vol. 73, Issue 4 https://doi.org/10.1021/j100724a057	journal	April 1969
Reductions by monovalent zinc, cadmium, and nickel cations Meyerstein, Dan; Mulac, William A. The Journal of Physical Chemistry, Vol. 72, Issue 3 https://doi.org/10.1021/j100849a004	journal	March 1968
Reaction of the Hydrated Electron with Water ¹ Hart, Edwin J.; Gordon, Sheffield; Fielden, E. M. The Journal of Physical Chemistry, Vol. 70, Issue 1 https://doi.org/10.1021/j100873a023	journal	January 1966
The Pulse Radiolysis of Aqueous Solutions of Potassium Ferrocyanide ¹ Rabani, J.; Matheson, M. S. The Journal of Physical Chemistry, Vol. 70, Issue 3 https://doi.org/10.1021/j100875a025	journal	March 1966
The Reactivity of Metal Ions and Some Oxy Anions toward Hydrated Electrons ¹ Anbar, M.; Hart, Edwin J. The Journal of Physical Chemistry, Vol. 69, Issue 3 https://doi.org/10.1021/j100887a048	journal	March 1965
Redox potentials of free radicals. I. Simple organic radicals Rao, P. S.; Hayon, E. Journal of the American Chemical Society, Vol. 96, Issue 5 https://doi.org/10.1021/ja00812a004	journal	March 1974
Hydration and Water Exchange of Zinc(II) Ions. Application of Density Functional Theory Hartmann, Michael; Clark, Timothy; van Eldik, Rudi Journal of the American Chemical Society, Vol. 119, Issue 33 https://doi.org/10.1021/ja970483f	journal	August 1997
Solvation Model Based on Weighted Solvent Accessible Surface Area Wang, Junmei; Wang, Wei; Huo, Shuanghong The Journal of Physical Chemistry B, Vol. 105, Issue 21 https://doi.org/10.1021/jp0102318	journal	May 2001
Infrared Spectroscopy of Solvation in Small Zn ⁺ (H ₂ O) _n Complexes Bandyopadhyay, Biswajit; Reishus, Kimberly N.; Duncan, Michael A. The Journal of Physical Chemistry A, Vol. 117, Issue 33 https://doi.org/10.1021/jp4046676	journal	July 2013
Raman Spectral Studies of Aqueous Zinc Nitrate Solution at High Temperatures and at a High Pressure of 30 MPa Ikushima, Yutaka; Saito, Norio; Arai, Masahiko The Journal of Physical Chemistry B, Vol. 102, Issue 16 https://doi.org/10.1021/jp980458b	journal	March 1998
Ultraviolet charge-transfer-to-solvent spectroscopy of halide and hydroxide ions in subcritical and supercritical water Marin, Timothy W.; Janik, Ireneusz; Bartels, David M. Physical Chemistry Chemical Physics, Vol. 21, Issue 44 https://doi.org/10.1039/C9CP03805A	journal	January 2019
One-electron redox kinetics of aqueous transition metal couples Zn ^2+/+ , Co ^2+/+ , and Ni ^2+/+ using pulse radiolysis Lisovskaya, Alexandra; Kanjana, Kotchaphan; Bartels, David M. Physical Chemistry Chemical Physics, Vol. 22, Issue 34 https://doi.org/10.1039/D0CP03214J	journal	January 2020
Long-range corrected hybrid density functionals with damped atom–atom dispersion corrections Chai, Jeng-Da; Head-Gordon, Martin Physical Chemistry Chemical Physics, Vol. 10, Issue 44 https://doi.org/10.1039/b810189b	journal	January 2008
Polarogram of the free hydrogen atom and of some simple organic radicals Toffel, P.; Henglein, A. Faraday Discussions of the Chemical Society, Vol. 63 https://doi.org/10.1039/dc9776300124	journal	January 1977
Pulse radiolysis study of monovalent cadmium, cobalt, nickel and zinc in aqueous solution. Part 1.—Formation and decay of the monovalent ions Buxton, George V.; Sellers, Robin M. Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 71, Issue 0 https://doi.org/10.1039/f19757100558	journal	January 1975
Pulse radiolysis study of monovalent cadmium, cobalt, nickel and zinc in aqueous solution. Part 2.—Reactions of the monovalent ions Buxton, George V.; Sellers, Robin M.; McCracken, David R. Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 72, Issue 0 https://doi.org/10.1039/f19767201464	journal	January 1976
Re-evaluation of the thiocyanate dosimeter for pulse radiolysis Buxton, George V.; Stuart, Craig R. Journal of the Chemical Society, Faraday Transactions, Vol. 91, Issue 2 https://doi.org/10.1039/ft9959100279	journal	January 1995
Polarization consistent basis sets: Principles Jensen, Frank The Journal of Chemical Physics, Vol. 115, Issue 20 https://doi.org/10.1063/1.1413524	journal	November 2001
Polarization consistent basis sets. II. Estimating the Kohn–Sham basis set limit Jensen, Frank The Journal of Chemical Physics, Vol. 116, Issue 17 https://doi.org/10.1063/1.1465405	journal	May 2002
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen Dunning, Thom H. The Journal of Chemical Physics, Vol. 90, Issue 2 https://doi.org/10.1063/1.456153	journal	January 1989
Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (⋅OH/⋅O ⁻ in Aqueous Solution Buxton, George V.; Greenstock, Clive L.; Helman, W. Phillips Journal of Physical and Chemical Reference Data, Vol. 17, Issue 2 https://doi.org/10.1063/1.555805	journal	April 1988
Chemical Kinetic Data Base for Combustion Chemistry. Part 3: Propane Tsang, Wing Journal of Physical and Chemical Reference Data, Vol. 17, Issue 2 https://doi.org/10.1063/1.555806	journal	April 1988
Laser Flash Photolysis and Photoinactivation of Subtilisin bpn' Blum, Aleksander; Grossweiner, Leonard I. Photochemistry and Photobiology, Vol. 36, Issue 6 https://doi.org/10.1111/j.1751-1097.1982.tb09480.x	journal	December 1982
Hydrated Electrons Produced by the Flash Photolysis of Co ⁺ , Ni ⁺ , Zn ⁺ , and Cd ⁺ Ions Basco, Norman; Vidyarthi, Sunil K.; Walker, David C. Canadian Journal of Chemistry, Vol. 52, Issue 2 https://doi.org/10.1139/v74-055	journal	January 1974
Competitive Measurement of Rate Constants for Hydroxyl Radical Reactions Using Radiolytic Hydroxylation of Benzoate. Motohashi, Noriko; Saito, Yutaka Chemical and Pharmaceutical Bulletin, Vol. 41, Issue 10 https://doi.org/10.1248/cpb.41.1842	journal	January 1993
Reactions of the Reducing Species in the Radiolysis of Aqueous Methanol Solutions Baxendale, J. H.; Dixon, R. S. Zeitschrift für Physikalische Chemie, Vol. 43, Issue 3_4 https://doi.org/10.1524/zpch.1964.43.3_4.161	journal	November 1964

Similar Records

Reduction of CO₂ by hydrated electrons in high temperature water

Journal Article · Mon Jan 28 19:00:00 EST 2019 · Radiation Physics and Chemistry (1993) · OSTI ID:1609021

Oxidizing radical formed by reaction of e/sub aq//sup -/ and SF/sub 6//sup 1/. [Kinetics]

Journal Article · Sun Aug 01 00:00:00 EDT 1976 · J. Phys. Chem.; (United States) · OSTI ID:7349390

Kinetics of the Temperature-Dependent e_aq^- and ·OH Radical Reactions with Cr(III) Ions in Aqueous Solutions

Journal Article · Tue Oct 24 20:00:00 EDT 2023 · ChemPhysChem · OSTI ID:2228293

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
Physics

Reactivity of Zn+aq in high-temperature water radiolysis

Citation Formats

References (43)

Similar Records

Related Subjects

Reactivity of Zn⁺_aq in high-temperature water radiolysis