Citation: XIA Xiang-Lai, LI Lin-Yan, GUO Fang, SU Wei, LIU Yan, CHEN Xiao-Mou, PAN She-Qi. Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x[J]. Acta Physico-Chimica Sinica, ;2015, 31(9): 1810-1814. doi: 10.3866/PKU.WHXB201507203 shu

Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x

XIA Xiang-Lai ^1,2 ,
LI Lin-Yan ^2, ,
GUO Fang ^1, ,
SU Wei ³ ,
LIU Yan ³ ,
CHEN Xiao-Mou ³ ,
PAN She-Qi ³

1.
1 College of Chemistry, Liaoning University, Shenyang 110036, P. R. China;
2 Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, P. R. China;
3 China Academy of Engineering Physics, Mianyang 621900, Sichuan Province, P. R. China

Received Date: 26 March 2015
Available Online: 20 July 2015
Fund Project: 国家自然科学基金委员会和中国工程物理研究院联合基金(11176014) (11176014)国家自然科学基金(21471088)资助项目 (21471088)

Polycrystalline samples of (Gd_1-xCe_x)₂Zr₂O_7+x (0 ≤ x ≤ 0.7) were synthesized by solid-state reaction using NaF as a flux at 1000 ℃ to simulate Pu-immobilization in the Gd₂Zr₂O₇ matrix. Phase transformation and variation of the thermal expansion coefficients (TECs) and thermal conductivities (TCs) of the samples with temperature and composition were investigated. Powder X-ray diffraction (XRD) patterns show that pure Gd₂Zr₂O₇ has a weakly ordered pyrochlore structure, whereas Ce-containing samples (i.e., the Pu-simulated solidified samples) exhibit a defect fluorite structure even if x is as low as 0.1. When x reaches 0.7, the XRD peaks of these samples widen. In the Ce 3d X-ray photoelectron spectrum (XPS) of (Gd_1-xCe_x)₂Zr₂O_7+x there are six peaks located at binding energies of 881.7, 888.1, 897.8, 900.4, 907.1, and 916.1 eV, which are almost the same as the peaks of CeO2. The Ce 3d XPS reveals that the Ce species in (Gd_1-xCe_x)₂Zr₂O_7+x are tetravalent. The TECs of (Gd_1-xCe_x)₂Zr₂O_7+x (0 ≤ x ≤ 0.7) generally increase with increasing temperature. At the same temperature, the TECs and TCs exhibit the same variation trend with the composition of the simulated solidified forms: they decrease from x = 0 to 0.1 and then linearly increase from x = 0.1 to 0.7.
- Immobilization of nuclear waste,
- Pyrochlore structure,
- Defect fluorite structure,
- Thermal expansion coefficient,
- Thermal conductivity
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Simulation of the Immobilization of Pu in the Gd2Zr2O7 Matrix by Investigating the Thermophysical Properties of (Gd1-xCex)2Zr2O7+x

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Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x