Synthesis and characterisation of Ca1-xCexZrTi2-2xCr2xO7: Analogue zirconolite wasteform for the immobilisation of stockpiled UK plutonium

被引：34

作者：

Blackburn, Lewis R. ^{[1
]}

Sun, Shi-Kuan ^{[1
]}

Lawson, Sebastian M. ^{[1
]}

Gardner, Laura J. ^{[1
]}

Ding, Hao ^{[1
]}

Corkhill, Claire L. ^{[1
]}

Maddrell, Ewan R. ^{[2
]}

Stennett, Martin C. ^{[1
]}

Hyatt, Neil C. ^{[1
]}

机构：

[1] Univ Sheffield, Dept Mat Sci & Engn, Immobilisat Sci Lab, Sir Robert Hadfield Bldg,Mappin St, Sheffield S1 3JD, S Yorkshire, England

[2] Natl Nucl Lab, Workington CA14 3YQ, Cumbria, England

来源：

JOURNAL OF THE EUROPEAN CERAMIC SOCIETY | 2020年 / 40卷 / 15期

基金：

英国工程与自然科学研究理事会;

关键词：

Zirconolite; Immobilisation; Plutonium; Surrogate; Wasteform; X-RAY-DIFFRACTION; CAZRTI2O7; BEHAVIOR;

D O I：

10.1016/j.jeurceramsoc.2020.05.066

中图分类号：

TQ174 [陶瓷工业]; TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

A series of Ca1-xCexZrTi2-2xCr2xO7 zirconolite ceramics (0 <= x <= 0.35) were reactively sintered in air at 1350 degrees C for 20 h. Single phase zirconolite-2M was formed for x <= 0.15, with Cr2O3 and an undesirable Ce-bearing perovskite phase present above x = 0.20. Electron diffraction analysis confirmed that the zirconolite-2M polytype was maintained over the solid solution. X-ray absorption near edge structure (XANES) data determined that between 10-20% Ce was speciated as Ce3+, and Cr was present uniformly as Cr3+ with near edge features consistent with occupation of octahedral sites within the zirconolite-2M structure. A sample corresponding to x = 0.20 was processed by reactive spark plasma sintering (RSPS), with a rapid processing time of less than 1 h. XANES data confirmed complete reduction to Ce3+ during RSPS, promoting the formation of a Ce-bearing perovskite, comprising 19.3 +/- 0.4 wt. % of the phase assemblage.

引用

页码：5909 / 5919

页数：11

共 36 条

[1] REEVALUATION OF X-RAY ATOMIC ENERGY LEVELS [J].

BEARDEN, JA ;

BURR, AF .

REVIEWS OF MODERN PHYSICS, 1967, 39 (01) :125-&

[2]

Begg B., 1996, MRS Online Proceedings Library (OPL), V465, P333

[3]

Begg BD, 1998, MATER RES SOC SYMP P, V506, P79

[4] The incorporation of plutonium and neptunium in zirconolite and perovskite [J].

Begg, BD ;

Vance, ER ;

Conradson, SD .

JOURNAL OF ALLOYS AND COMPOUNDS, 1998, 271 :221-226

[5] The use of surrogates in waste immobilization studies: A case study of plutonium [J].

Bingham, Paul A. ;

Hand, Russell J. ;

Stennett, Martin C. ;

Hyatt, Neil C. ;

Harrison, Mike T. .

SCIENTIFIC BASIS FOR NUCLEAR WASTE MANAGEMENT XXXI, 2008, 1107 :421-+

[6] First-principles calculations of X-ray absorption spectra at the K-edge of 3d transition metals: an electronic structure analysis of the pre-edge [J].

Cabaret, Delphine ;

Bordage, Amelie ;

Juhin, Amelie ;

Arfaoui, Mounir ;

Gaudry, Emilie .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2010, 12 (21) :5619-5633

[7] Microstructures of Melt-Processed and Spark Plasma Sintered Ceramic Waste Forms [J].

Clark, B. M. ;

Tumurugoti, P. ;

Sundaram, S. K. ;

Amoroso, J. W. ;

Marra, J. C. ;

Brinkman, K. S. .

METALLURGICAL AND MATERIALS TRANSACTIONS E-MATERIALS FOR ENERGY SYSTEMS, 2014, 1 (04) :341-348

[8] Polymorphic Transitions in Cerium-Substituted Zirconolite (CaZrTi2O7) [J].

Clark, Braeden M. ;

Sundaram, S. K. ;

Misture, Scott T. .

SCIENTIFIC REPORTS, 2017, 7

[9] Analysis and structural determination of Nd-substituted zirconolite-4M [J].

Coelho, AA ;

Cheary, RW ;

Smith, KL .

JOURNAL OF SOLID STATE CHEMISTRY, 1997, 129 (02) :346-359

[10] Nuclear waste disposal-pyrochlore (A2B2O7):: Nuclear waste form for the immobilization of plutonium and "minor" actinides [J].

Ewing, RC ;

Weber, WJ ;

Lian, J .

JOURNAL OF APPLIED PHYSICS, 2004, 95 (11) :5949-5971

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