Thermal annealing of natural, radiation-damaged pyrochlore

J 2017

Thermal annealing of natural, radiation-damaged pyrochlore

ZIETLOW, Peter, Tobias BEIRAU, Boriana MIHAILOVA, Lee GROAT, Thomas CHUDY et. al.

Basic information

Original name

Thermal annealing of natural, radiation-damaged pyrochlore

Authors

ZIETLOW, Peter (276 Germany), Tobias BEIRAU (276 Germany), Boriana MIHAILOVA (643 Russian Federation), Lee GROAT (124 Canada), Thomas CHUDY (124 Canada), Anna SHELYUG (840 United States of America), Alexandra NAVROTSKY (840 United States of America), Rodney EWING (840 United States of America), Jochen SCHLUTER (276 Germany), Radek ŠKODA (203 Czech Republic, guarantor, belonging to the institution) and Ullrich BISMAYER (276 Germany)

Edition

ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS, BERLIN, WALTER DE GRUYTER GMBH, 2017, 2194-4946

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10504 Mineralogy

Country of publisher

Germany

Confidentiality degree

není předmětem státního či obchodního tajemství

Impact factor

Impact factor: 1.263

RIV identification code

RIV/00216224:14310/17:00100326

Organization unit

Faculty of Science

DOI

http://dx.doi.org/10.1515/zkri-2016-1965

UT WoS

000394243800004

Keywords in English

actinide impurities; metamict; pyrochlore; radiation damage; Raman spectroscopy

Abstract

V originále

Radiation damage in minerals is caused by the a-decay of incorporated radionuclides, such as U and Th and their decay products. The effect of thermal annealing (400-1000 K) on radiation-damaged pyro-chlores has been investigated by Raman scattering, X-ray powder diffraction (XRD), and combined differential scanning calorimetry/thermogravimetry (DSC/TG). The analysis of three natural radiation-damaged pyrochlore samples from Miass/Russia [6.4 wt% Th, 23.1 10(18) alpha-decay events per gram (dpg)], Panda Hill/Tanzania (1.6 wt% Th, 1.6 10(18) dpg), and Blue River/Canada (10.5 wt% U, 115.4 10(18) dpg), are compared with a crystalline refer-ence pyrochlore from Schelingen (Germany). The type of structural recovery depends on the initial degree of radiation damage (Panda Hill 28 %, Blue River 85 % and Miass 100 % according to XRD), as the recrystallization tem-perature increases with increasing degree of amorphization. Raman spectra indicate reordering on the local scale during annealing-induced recrystallization. As Raman modes around 800 cm(-1) are sensitive to radiation damageM. T. Vandenborre, E. Husson, Comparison of the force field in various pyrochlore families. I. The A(2)B O-2 (7) oxides. J. Solid State Chem. 1983, 50, 362, S. Moll, G. Sattonnay, L. Thome, J. Jagielski, C. Decorse, P. Simon, I. Monnet, W. J. Weber, Irradiation damage in Gd-2 Ti-2 O-7 single crystals: Ballistic versus ionization processes. Phys. Rev. 2011, 84, 64115.), the degree of local order was deduced from the ratio of the integrated intensities of the sum of the Raman bands between 605 and 680 cm (1) divided by the sum of the integrated intensities of the bands between 810 and 860 cm(-1). The most radiation damaged pyrochlore (Miass) shows an abrupt recovery of both, its short-(Raman) and long-range order (X-ray) between 800 and 850 K, while the weakly damaged pyrochlore (Panda Hill) begins to recover at considerably lower temperatures (near 500 K), extending over a temperature range of ca. 300 K, up to 800 K (Raman). The pyrochlore from Blue River shows in its initial state an amorphous X-ray diffraction pattern superimposed by weak Bragg-maxima that indicates the existence of ordered regions in a damaged matrix. In con-trast to the other studied pyrochlores, Raman spectra of the Blue River sample show the appearance of local modes above 560 K between 700 and 800 cm(-1) resulting from its high content of U and Ta impurities. DSC measurements confirmed the observed structural recovery upon anneal-ing. While the annealing-induced ordering of Panda Hill begins at a lower temperature (ca. 500 K) the recovery of the highly-damaged pyrochlore from Miass occurs at 800 K. The Blue-River pyrochlore shows a multi-step recovery which is similarly seen by XRD. Thermogravi-metry showed a continuous mass loss on heating for all radiation-damaged pyrochlores (Panda Hill ca. 1 %, Blue River ca. 1.5 %, Miass ca. 2.9 %).

Links

MUNI/A/1316/2015, interní kód MU

Name: Geologické, geodynamické a environmentální procesy východního okraje Českého masívu (Acronym: Geodyn)

Investor: Masaryk University, Category A

Citovat

ZIETLOW, Peter, Tobias BEIRAU, Boriana MIHAILOVA, Lee GROAT, Thomas CHUDY, Anna SHELYUG, Alexandra NAVROTSKY, Rodney EWING, Jochen SCHLUTER, Radek ŠKODA and Ullrich BISMAYER. Thermal annealing of natural, radiation-damaged pyrochlore. ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS. BERLIN: WALTER DE GRUYTER GMBH, 2017, vol. 232, 1-3, p. 25-38. ISSN 2194-4946. Available from: https://dx.doi.org/10.1515/zkri-2016-1965.

@article{1410983,
   author = {Zietlow, Peter and Beirau, Tobias and Mihailova, Boriana and Groat, Lee and Chudy, Thomas and Shelyug, Anna and Navrotsky, Alexandra and Ewing, Rodney and Schluter, Jochen and Škoda, Radek and Bismayer, Ullrich},
   article_location = {BERLIN},
   article_number = {1-3},
   doi = {http://dx.doi.org/10.1515/zkri-2016-1965},
   keywords = {actinide impurities; metamict; pyrochlore; radiation damage; Raman spectroscopy},
   language = {eng},
   issn = {2194-4946},
   journal = {ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS},
   title = {Thermal annealing of natural, radiation-damaged pyrochlore},
   volume = {232},
   year = {2017}
}

TY  - JOUR
ID  - 1410983
AU  - Zietlow, Peter - Beirau, Tobias - Mihailova, Boriana - Groat, Lee - Chudy, Thomas - Shelyug, Anna - Navrotsky, Alexandra - Ewing, Rodney - Schluter, Jochen - Škoda, Radek - Bismayer, Ullrich
PY  - 2017
TI  - Thermal annealing of natural, radiation-damaged pyrochlore
JF  - ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS
VL  - 232
IS  - 1-3
SP  - 25-38
EP  - 25-38
PB  - WALTER DE GRUYTER GMBH
SN  - 21944946
KW  - actinide impurities
KW  - metamict
KW  - pyrochlore
KW  - radiation damage
KW  - Raman spectroscopy
N2  - Radiation damage in minerals is caused by the a-decay of incorporated radionuclides, such as U and Th and their decay products. The effect of thermal annealing (400-1000 K) on radiation-damaged pyro-chlores has been investigated by Raman scattering, X-ray powder diffraction (XRD), and combined differential scanning calorimetry/thermogravimetry (DSC/TG). The analysis of three natural radiation-damaged pyrochlore samples from Miass/Russia [6.4 wt% Th, 23.1 10(18) alpha-decay events per gram (dpg)], Panda Hill/Tanzania (1.6 wt% Th, 1.6 10(18) dpg), and Blue River/Canada (10.5 wt% U, 115.4 10(18) dpg), are compared with a crystalline refer-ence pyrochlore from Schelingen (Germany). The type of structural recovery depends on the initial degree of radiation damage (Panda Hill 28 %, Blue River 85 % and Miass 100 % according to XRD), as the recrystallization tem-perature increases with increasing degree of amorphization. Raman spectra indicate reordering on the local scale during annealing-induced recrystallization. As Raman modes around 800 cm(-1) are sensitive to radiation damageM. T. Vandenborre, E. Husson, Comparison of the force field in various pyrochlore families. I. The A(2)B O-2 (7) oxides. J. Solid State Chem. 1983, 50, 362, S. Moll, G. Sattonnay, L. Thome, J. Jagielski, C. Decorse, P. Simon, I. Monnet, W. J. Weber, Irradiation damage in Gd-2 Ti-2 O-7 single crystals: Ballistic versus ionization processes. Phys. Rev. 2011, 84, 64115.), the degree of local order was deduced from the ratio of the integrated intensities of the sum of the Raman bands between 605 and 680 cm (1) divided by the sum of the integrated intensities of the bands between 810 and 860 cm(-1). The most radiation damaged pyrochlore (Miass) shows an abrupt recovery of both, its short-(Raman) and long-range order (X-ray) between 800 and 850 K, while the weakly damaged pyrochlore (Panda Hill) begins to recover at considerably lower temperatures (near 500 K), extending over a temperature range of ca. 300 K, up to 800 K (Raman). The pyrochlore from Blue River shows in its initial state an amorphous X-ray diffraction pattern superimposed by weak Bragg-maxima that indicates the existence of ordered regions in a damaged matrix. In con-trast to the other studied pyrochlores, Raman spectra of the Blue River sample show the appearance of local modes above 560 K between 700 and 800 cm(-1) resulting from its high content of U and Ta impurities. DSC measurements confirmed the observed structural recovery upon anneal-ing. While the annealing-induced ordering of Panda Hill begins at a lower temperature (ca. 500 K) the recovery of the highly-damaged pyrochlore from Miass occurs at 800 K. The Blue-River pyrochlore shows a multi-step recovery which is similarly seen by XRD. Thermogravi-metry showed a continuous mass loss on heating for all radiation-damaged pyrochlores (Panda Hill ca. 1 %, Blue River ca. 1.5 %, Miass ca. 2.9 %).
ER  -

ZIETLOW, Peter, Tobias BEIRAU, Boriana MIHAILOVA, Lee GROAT, Thomas CHUDY, Anna SHELYUG, Alexandra NAVROTSKY, Rodney EWING, Jochen SCHLUTER, Radek ŠKODA and Ullrich BISMAYER. Thermal annealing of natural, radiation-damaged pyrochlore. \textit{ZEITSCHRIFT FUR KRISTALLOGRAPHIE-CRYSTALLINE MATERIALS}. BERLIN: WALTER DE GRUYTER GMBH, 2017, vol.~232, 1-3, p.~25-38. ISSN~2194-4946. Available from: https://dx.doi.org/10.1515/zkri-2016-1965.

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