Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations

I. Denden; F. Poineau; M. L. Schlegel; J. Roques; P. Lorenzo Solari; G. Blain; K. R. Czerwinski; R. Essehli; J. Barbet; M. Fattahi

doi:10.1021/jp404967f

Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations

I. Denden, F. Poineau, M. L. Schlegel, J. Roques, P. Lorenzo Solari, G. Blain, K. R. Czerwinski, R. Essehli, J. Barbet, M. Fattahi

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Abstract

The effect of α-radiolysis on the behavior of heptavalent technetium has been investigated in 13 and 18 M H₂SO₄. Irradiation experiments were performed using α-particles (⁴He²⁺, E = 68 MeV) generated by the ARRONAX cyclotron. UV-visible and X-ray absorption fine structure spectroscopic studies indicate that Tc(VII) is reduced to Tc(V) under α-irradiation. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements are consistent with the presence of mononuclear technetium sulfate complexes. Experimental results and density functional calculations show the formation of [TcO(HSO₄)₃(H ₂O)(OH)]^- and/or [TcO(HSO₄)₃(H ₂O)₂] and [Tc(HSO₄)₃(SO ₄)(H₂O)] and/or [Tc(HSO₄)₃(SO ₄)(OH)]^- for 13 and 18 M H₂SO₄, respectively.

Original language	English
Pages (from-to)	1568-1575
Number of pages	8
Journal	Journal of Physical Chemistry A
Volume	118
Issue number	9
DOIs	https://doi.org/10.1021/jp404967f
State	Published - Mar 6 2014
Externally published	Yes

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Denden, I., Poineau, F., Schlegel, M. L., Roques, J., Solari, P. L., Blain, G., Czerwinski, K. R., Essehli, R., Barbet, J., & Fattahi, M. (2014). Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations. Journal of Physical Chemistry A, 118(9), 1568-1575. https://doi.org/10.1021/jp404967f

@article{b06f7e74eeb040d7b7f6cccd9d9f810a,

title = "Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations",

abstract = "The effect of α-radiolysis on the behavior of heptavalent technetium has been investigated in 13 and 18 M H2SO4. Irradiation experiments were performed using α-particles (4He2+, E = 68 MeV) generated by the ARRONAX cyclotron. UV-visible and X-ray absorption fine structure spectroscopic studies indicate that Tc(VII) is reduced to Tc(V) under α-irradiation. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements are consistent with the presence of mononuclear technetium sulfate complexes. Experimental results and density functional calculations show the formation of [TcO(HSO4)3(H 2O)(OH)]- and/or [TcO(HSO4)3(H 2O)2] and [Tc(HSO4)3(SO 4)(H2O)] and/or [Tc(HSO4)3(SO 4)(OH)]- for 13 and 18 M H2SO4, respectively.",

author = "I. Denden and F. Poineau and Schlegel, {M. L.} and J. Roques and Solari, {P. Lorenzo} and G. Blain and Czerwinski, {K. R.} and R. Essehli and J. Barbet and M. Fattahi",

year = "2014",

month = mar,

day = "6",

doi = "10.1021/jp404967f",

language = "English",

volume = "118",

pages = "1568--1575",

journal = "Journal of Physical Chemistry A",

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publisher = "American Chemical Society",

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}

Denden, I, Poineau, F, Schlegel, ML, Roques, J, Solari, PL, Blain, G, Czerwinski, KR, Essehli, R, Barbet, J & Fattahi, M 2014, 'Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations', Journal of Physical Chemistry A, vol. 118, no. 9, pp. 1568-1575. https://doi.org/10.1021/jp404967f

Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations. / Denden, I.; Poineau, F.; Schlegel, M. L. et al.
In: Journal of Physical Chemistry A, Vol. 118, No. 9, 06.03.2014, p. 1568-1575.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Behavior of heptavalent technetium in sulfuric acid under α-irradiation

T2 - Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations

AU - Denden, I.

AU - Poineau, F.

AU - Schlegel, M. L.

AU - Roques, J.

AU - Solari, P. Lorenzo

AU - Blain, G.

AU - Czerwinski, K. R.

AU - Essehli, R.

AU - Barbet, J.

AU - Fattahi, M.

PY - 2014/3/6

Y1 - 2014/3/6

N2 - The effect of α-radiolysis on the behavior of heptavalent technetium has been investigated in 13 and 18 M H2SO4. Irradiation experiments were performed using α-particles (4He2+, E = 68 MeV) generated by the ARRONAX cyclotron. UV-visible and X-ray absorption fine structure spectroscopic studies indicate that Tc(VII) is reduced to Tc(V) under α-irradiation. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements are consistent with the presence of mononuclear technetium sulfate complexes. Experimental results and density functional calculations show the formation of [TcO(HSO4)3(H 2O)(OH)]- and/or [TcO(HSO4)3(H 2O)2] and [Tc(HSO4)3(SO 4)(H2O)] and/or [Tc(HSO4)3(SO 4)(OH)]- for 13 and 18 M H2SO4, respectively.

AB - The effect of α-radiolysis on the behavior of heptavalent technetium has been investigated in 13 and 18 M H2SO4. Irradiation experiments were performed using α-particles (4He2+, E = 68 MeV) generated by the ARRONAX cyclotron. UV-visible and X-ray absorption fine structure spectroscopic studies indicate that Tc(VII) is reduced to Tc(V) under α-irradiation. Extended X-ray absorption fine structure (EXAFS) spectroscopy measurements are consistent with the presence of mononuclear technetium sulfate complexes. Experimental results and density functional calculations show the formation of [TcO(HSO4)3(H 2O)(OH)]- and/or [TcO(HSO4)3(H 2O)2] and [Tc(HSO4)3(SO 4)(H2O)] and/or [Tc(HSO4)3(SO 4)(OH)]- for 13 and 18 M H2SO4, respectively.

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SN - 1089-5639

VL - 118

SP - 1568

EP - 1575

JO - Journal of Physical Chemistry A

JF - Journal of Physical Chemistry A

IS - 9

ER -

Behavior of heptavalent technetium in sulfuric acid under α-irradiation: Structural determination of technetium sulfate complexes by X-ray absorption spectroscopy and first principles calculations

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