Chemical durability and surface alteration of lanthanide zirconates (A2Zr2O7: A = La-Yb)
Source abstract
Abstract
Abstract Chemical durability of lanthanide zirconates (A2Zr2O7) (A = La-Yb) under near-field environments is important for evaluating their application as potential nuclear waste forms. In this work, A2Zr2O7 (A = La-Yb) are synthesized by spark plasma sintering with controlled microstructure and their chemical durability are evaluated in a nitric acid solution (pH = 1). Scanning transmission electron microscopy analysis reveals an amorphous passivation film either enriched with Zr or lanthanide. The complex chemistry of the passivation films can be correlated with a transition in corrosion mechanisms from a preferential release of lanthanide in La2Zr2O7 to a preferential release of Zr in Er2Zr2O7 and Yb2Zr2O7. These results suggest a dominant mechanism of incongruent dissolution and surface reorganization for the formation of passivation films. Strong correlations are identified between the leaching rates and cation ionic size, ionic potential, electronegativity differences between A-site cation and Zr, and bonding valence sum of oxygen, suggesting important impacts of structural and bonding characteristics in controlling chemical durability of lanthanide zirconates.
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Research context
OpenAlex topics: Nuclear materials and radiation effects · Electronic and Structural Properties of Oxides · Ferroelectric and Piezoelectric Materials
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References (59)
Show source-provided references
1. Gd2Zr2O7 and Nd2Zr2O7 pyrochlore prepared by aqueous chemical synthesis10.1016/j.jeurceramsoc.2013.05.011 ↗
2. Synthesis and characterization of Gd2Zr2O7 defect fluorite oxide nanoparticles via a homogeneous precipitation-solvothermal method10.1039/C7RA11019G ↗
3. Hot corrosion behaviors of gas tunnel type plasma sprayed La2Zr2O7 thermal barrier coatings10.1016/j.jeurceramsoc.2011.10.049 ↗
4. From fluorite to pyrochlore: characterization of local and average structural of neodymium zirconate, Nd2Zr2O710.1016/j.jssc.2013.07.001 ↗
5. Zirconolite rich titanate ceramics for immobilization of actinides-waste form/HIP can interactions and chemical durability10.1016/j.jnucmat.2009.09.019 ↗
6. Monitoring the microstructural evolution of Nd2Zr2O7 pyrochlore during dissolution at 90°C in 4M HCl: implications regarding the evaluation of the chemical durability10.1016/j.jnucmat.2017.09.029 ↗
7. Nuclear waste disposal-pyrochlore (A2B2O7): nuclear waste form for the immobilization of plutonium and minor actinides10.1063/1.1707213 ↗
8. Immobilization of high-level nuclear reactor wastes in SYNROC: a current appraisal10.1016/0191-815X(81)90055-3 ↗
9. Investigation of pyrochlore-based U-Bearing ceramic nuclear waste: uranium leaching test and TEM observation10.1021/es030582v ↗
10. Aqueous alteration of nearly pure Nd-doped zirconolite (Ca0.8Nd0.2ZrTi1.8Al0.2O7), a passivating layer control10.1016/j.apgeochem.2004.10.006 ↗
11. Zirconate pyrochlore as a transmutation target: thermal behaviour and radiation resistance against fission fragment impact10.1016/S0022-3115(03)00134-X ↗
12. Radiation stability of gadolinium zirconate: a waste form for plutonium disposition10.1557/JMR.1999.0606 ↗
13. Heavy-ion irradiation effects on structures and acid dissolution of pyrochlores10.1016/S0022-3115(00)00708-X ↗
14. Dissolution of ZrO2 based pyrochlores in the acid pH range: a macroscopic and electron microscopy study10.1016/j.apgeochem.2014.06.014 ↗
15. Energetics of defect fluorite and pyrochlore phases in lanthanum and gadolinium hafnates10.1111/j.1551-2916.2007.01592.x ↗
16. Self-propagating high temperature synthesis of ZrO2 incorporated Gd2Ti2O7 pyrochlore10.1007/s40145-017-0254-0 ↗
17. Design and fabrication of Gd2Zr2O7 based waste forms for U3O8 immobilization in high capacity10.1007/s10853-016-9831-9 ↗
18. Synthesis and dissolution kinetics of zirconia based ceramics10.1016/j.pnucene.2013.07.020 ↗
19. Glass matrix/pyrochlore phase composites for nuclear wastes encapsulation10.1023/A:1023242702644 ↗
20. Gd2Zr2O7 pyrochlore: potential host matrix for some constituents of thoria based reactor’s waste10.1016/j.jnucmat.2010.08.042 ↗
21. Self-propagating synthesis of Y2-xNdxTi2O7 pyrochlore and its aqueous durability as nuclear waste form10.1016/j.scriptamat.2017.12.020 ↗
22. Pyrochlore riched Synroc as a host for immobilization of actinides
23. Pyrochlore based glass ceramics for the immobilization of actinide rich nuclear wastes: from concept to reality10.1016/j.jnucmat.2012.08.035 ↗
24. New perspective on the fluorite-pyrochlore phase transition in La2Zr2O7 and the importance of local oxygen related disordered states
25. The structural transformation from the pyrochlore structure, A2B2O7, to the fluorite structure, AO2, studied by Raman spectroscopy and defect chemistry modeling10.1006/jssc.2000.9142 ↗
26. Disorder in pyrochlore oxides10.1111/j.1151-2916.2000.tb01484.x ↗
27. Structural and crystal chemical properties of rare-earth titanate pyrochlores10.1016/j.jallcom.2014.03.153 ↗
28. Radiation stability of gadolinium zirconate: a waste form for plutonium disposition10.1557/JMR.1999.0606 ↗
29. Phase stability and pressure dependence of defect formation in Gd2Ti2O7 and Gd2Zr2O7 pyrochlores10.1103/PhysRevLett.100.045503 ↗
30. From fluorite to pyrochlore: characterization of local and average structural of neodymium zirconate, Nd2Zr2O710.1016/j.jssc.2013.07.001 ↗
31. Structural and electrical properties of layered pervoskite type Pr2Ti2O7: experimental and theoretical investigations10.1039/C5TC00242G ↗
32. Flux synthesis and chemical stability of Nd and Ce co-doped (Gd1-xNdx)(Zr1-xCex)2O7 (0≤x≤1) pyrochlore ceramics for nuclear waste forms10.1016/j.ceramint.2017.09.121 ↗
33. Synthesis and conductivity of Yb2Ti2O7 nanoceramics10.1016/j.ssi.2005.04.038 ↗
34. Order disorder phase transitions and high temperature oxide ion conductivity of Er2+xTi2-xO7-x (x=0,0.096)10.1016/j.materresbull.2006.07.011 ↗
35. Electrical conductivity anomaly around fluorite pyrochlore phase boundary10.1016/S0167-2738(02)00874-3 ↗
36. Chemical durability of yitria-stabilized zirconia for highly concentrated tru wastes10.1557/PROC-608-393 ↗
37. Rapid synthesis and chemical durability of Gd2Zr2-xCexO7 via SPS for nuclear waste forms10.1016/j.ceramint.2018.08.018 ↗
38. Durability of an La2Zr2O7 waste form containing various amounts of simulated HLW elements10.1016/0022-3115(93)90039-2 ↗
39. Crystalline materials for actinide immobilization. Imperial College Press
40. Cubic zirconia as a candidate waste form for actinides: dissolution studies10.1007/BF01730301 ↗
41. Durability of zirconium containing ceramic waste forms in water10.1111/j.1151-2916.1991.tb06942.x ↗
42. Behavior of 238Pu-doped ceramics based on cubic zirconia and pyrochlore under radiation damage10.1080/00223131.2002.10875571 ↗
43. Behavior of 238Pu-doped cubic zirconia under self-irradiation
44. Leaching of plutonium from old samples of single ceramics based on Zr0.79Gd0.14Pu0.04O1.93 and La0.9Pu0.1PO4 doped with 238Pu
45. Pyrochlore as nuclear waste form: actinide uptake and chemical stability
46. An attempt to correlate ion irradiation behaviour and chemical durability of titanate and zirconate based ceramics10.1016/j.nimb.2008.03.223 ↗
47. Nanometre-scale evidence for interfacial dissolution-reprecipitation control of silicate glass corrosion10.1038/nmat4172 ↗
48. Pyrochlore structural chemistry: predicting the lattice constant by the ionic radii and electronegativities of the constituting ions10.1111/j.1551-2916.2012.05115.x ↗
49. Synthesis and characterization of monoclinic rare earth titanates, RE2Ti2O7 (RE=La,Pr,Nd), by a modified SHS method using inorganic activator10.1007/s12034-008-0145-7 ↗
50. ASTM-C1308-08 · 2009
51. An evaluation of cement-based waste forms using the results of approximately two years of dynamic leaching10.1016/0191-815X(87)90007-6 ↗
52. A review of focused ion beam milling techniques for TEM specimen preparation10.1016/S0968-4328(99)00005-0 ↗
53. Crystal structure analysis of Ln2Zr2O7 (Ln=Eu and La) with a pyrochlore composition by high-temperature powder X-ray diffraction10.2109/jcersj2.16248 ↗
54. Order-disorder transition and unconventional thermal conductivities of the (Sm1-x,Ybx)2Zr2O7 series10.1111/j.1551-2916.2010.04113.x ↗
55. Evidence for dissolution-reprecipitation of apatite and preferential LREE mobility in carbonatite-derived late-stage hydrothermal processes10.2138/am-2016-5502CCBY ↗
56. Role and determining factor of substitutional defects on thermal conductivity: a study of La2(Zr1-xBx)2O7 (B=Hf,Ce, 0≤x≤0.5) pyrochlore solid solutions10.1016/j.actamat.2014.01.011 ↗
57. Electronegativity difference as a factor for evaluating the thermal stability of Al-rich metallic glasses10.1080/09500830802526596 ↗
58. Structural and bonding trends in Tin pyrochlore oxides10.1006/jssc.1997.7277 ↗
59. A systematic study of lanthanide titanates (A2Ti2O7) chemical durability: corrosion mechanisms and control parameters