A systematic investigation of the phase assemblage and microstructure of the zirconolite CaZr1-xCexTi2O7 system

被引：30

作者：

Blackburn, Lewis R. ^{[1
]}

Sun, Shikuan ^{[1
]}

Gardner, Laura J. ^{[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 S13JD, S Yorkshire, England

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

来源：

JOURNAL OF NUCLEAR MATERIALS | 2020年 / 535卷

基金：

英国工程与自然科学研究理事会;

关键词：

Cerium; Plutonium; Zirconolite; Immobilisation; Surrogate; Wasteform; Ceramic; X-RAY-DIFFRACTION; CRYSTAL-STRUCTURE; EVOLUTION; PLUTONIUM; CERIUM; CAZRTI2O7; RAMAN; ND;

D O I：

10.1016/j.jnucmat.2020.152137

中图分类号：

T [工业技术];

学科分类号：

08 ;

摘要：

A series of zirconolite ceramics with nominal stoichiometry CaZr1-xCexTi2O7 (0.0 <= x <= 0.4) were synthesised under oxidizing, inert and reducing conditions, by a conventional solid-state cold press and sinter method. The evolution of phase assemblage and microstructure were characterized by XRD, SEM-EDS, Ce-L-3 XANES and Raman spectroscopy techniques. It was determined that the relative yield of zirconolite-2M and zirconolite-4M polytypes, alongside secondary perovskite phases, was influenced by processing environment via the control of Ce3+/4+ speciation. Oxidizing conditions produced a mixture of zirconolite-2M and zirconolite-4M polytypes due to the formation of Ce4+. Inert and reducing conditions yielded predominantly zirconolite-2M and a Ce-bearing perovskite phase through favouring Ce3+ speciation. (C) 2020 The Authors. Published by Elsevier B.V.

引用

页数：11

共 33 条

[1]

[Anonymous], 2011, Management of the U.K.s Plutonium Stocks: A Consultation on the Long-Term Management of U.K. Owned Separated Civil Plutonium

[2] Synthesis and characterisation of brannerite compositions (U0.9Ce0.1)1-xMxTi2O6 (M = Gd3+, Ca2+) for the immobilisation of MOX residues [J].

Bailey, D. J. ;

Stennett, M. C. ;

Ravel, B. ;

Grolimund, D. ;

Hyatt, N. C. .

RSC ADVANCES, 2018, 8 (04) :2092-2099

[3]

Begg B.D., 2001, Materials Research Society Symposia Proceedings, V663, P1

[4]

Begg BD, 1997, MAT RES S C, V465, P333

[5] Zirconolite transformation under reducing conditions [J].

Begg, BD ;

Vance, ER ;

Hunter, BA ;

Hanna, JV .

JOURNAL OF MATERIALS RESEARCH, 1998, 13 (11) :3181-3190

[6]

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

[7] 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

[8]

Bingham P.A., 2008, MAT RES SOC S P, V1107

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

Clark, Braeden M. ;

Sundaram, S. K. ;

Misture, Scott T. .

SCIENTIFIC REPORTS, 2017, 7

[10] 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

← 1 2 3 4 →