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Article: Synchrotron X-ray Spectroscopy Investigation of the Ca1-xLnxZrTi2-x(Al,Fe)xO7 Zirconolite Ceramics (Ln=La, Nd, Gd, Ho, Yb)

TitleSynchrotron X-ray Spectroscopy Investigation of the Ca1-xLnxZrTi2-x(Al,Fe)xO7 Zirconolite Ceramics (Ln=La, Nd, Gd, Ho, Yb)
Authors
Keywordsnuclear waste
phase transformations
x-ray methods
zirconolite-2M
Issue Date2020
PublisherWiley-Blackwell Publishing, Inc. The Journal's web site is located at http://onlinelibrary.wiley.com/journal/10.1111/(ISSN)1551-2916
Citation
Journal of the American Ceramic Society, 2020, v. 103 n. 2, p. 1463-1475 How to Cite?
AbstractWhen incorporating actinides into zirconolite for high-level radioactive waste immobilization, Al3+ and Fe3+ ions generally act as charge compensators. In this study, we rationally designed a series of urn:x-wiley:00027820:media:jace16832:jace16832-math-0001 (Ln = La, Nd, Gd, Ho, Yb) to unravel the dopant solubility and evolutions of the crystalline phase and local environment of cations through synchrotron X-ray methods. It was found that single zirconolite phase is difficult to obtain and the fraction of perovskite have an increase with x from 0.1 to 0.9 in urn:x-wiley:00027820:media:jace16832:jace16832-math-0002. Formation of both zirconolite-2M and zirconolite-3O phases was observed in urn:x-wiley:00027820:media:jace16832:jace16832-math-0003 and urn:x-wiley:00027820:media:jace16832:jace16832-math-0004. Phase transformation from zirconolite-2M to 3O occurs at x = 0.7 for urn:x-wiley:00027820:media:jace16832:jace16832-math-0005 while x = 0.9 for urn:x-wiley:00027820:media:jace16832:jace16832-math-0006. The solubility of urn:x-wiley:00027820:media:jace16832:jace16832-math-0007 and urn:x-wiley:00027820:media:jace16832:jace16832-math-0008 to form single zirconolite-2M can reach to 0.9 f.u. and 0.7 f.u., respectively. The evolution of lattice parameters of zirconolite in urn:x-wiley:00027820:media:jace16832:jace16832-math-0009 is greatly related to the ionic radii of cations and substitution mechanism among the cations. X-ray absorption near edge spectroscopy revealed that Fe3+ ions replace both five- and six-coordinated Ti sites and the ratio of TiO5 to TiO6 decreases when increasing dopant concentration in the urn:x-wiley:00027820:media:jace16832:jace16832-math-0010. For the local environment of Zr4+, the major form is ZrO7 with a trace of ZrO8.
Persistent Identifierhttp://hdl.handle.net/10722/291162
ISSN
2023 Impact Factor: 3.5
2023 SCImago Journal Rankings: 0.819
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorJi, S-
dc.contributor.authorSu, M-
dc.contributor.authorLiao, C-
dc.contributor.authorMA, S-
dc.contributor.authorWang, Z-
dc.contributor.authorShih, K-
dc.contributor.authorChang, CK-
dc.contributor.authorLee, JF-
dc.contributor.authorChan, TS-
dc.contributor.authorLi, Y-
dc.date.accessioned2020-11-07T13:53:04Z-
dc.date.available2020-11-07T13:53:04Z-
dc.date.issued2020-
dc.identifier.citationJournal of the American Ceramic Society, 2020, v. 103 n. 2, p. 1463-1475-
dc.identifier.issn0002-7820-
dc.identifier.urihttp://hdl.handle.net/10722/291162-
dc.description.abstractWhen incorporating actinides into zirconolite for high-level radioactive waste immobilization, Al3+ and Fe3+ ions generally act as charge compensators. In this study, we rationally designed a series of urn:x-wiley:00027820:media:jace16832:jace16832-math-0001 (Ln = La, Nd, Gd, Ho, Yb) to unravel the dopant solubility and evolutions of the crystalline phase and local environment of cations through synchrotron X-ray methods. It was found that single zirconolite phase is difficult to obtain and the fraction of perovskite have an increase with x from 0.1 to 0.9 in urn:x-wiley:00027820:media:jace16832:jace16832-math-0002. Formation of both zirconolite-2M and zirconolite-3O phases was observed in urn:x-wiley:00027820:media:jace16832:jace16832-math-0003 and urn:x-wiley:00027820:media:jace16832:jace16832-math-0004. Phase transformation from zirconolite-2M to 3O occurs at x = 0.7 for urn:x-wiley:00027820:media:jace16832:jace16832-math-0005 while x = 0.9 for urn:x-wiley:00027820:media:jace16832:jace16832-math-0006. The solubility of urn:x-wiley:00027820:media:jace16832:jace16832-math-0007 and urn:x-wiley:00027820:media:jace16832:jace16832-math-0008 to form single zirconolite-2M can reach to 0.9 f.u. and 0.7 f.u., respectively. The evolution of lattice parameters of zirconolite in urn:x-wiley:00027820:media:jace16832:jace16832-math-0009 is greatly related to the ionic radii of cations and substitution mechanism among the cations. X-ray absorption near edge spectroscopy revealed that Fe3+ ions replace both five- and six-coordinated Ti sites and the ratio of TiO5 to TiO6 decreases when increasing dopant concentration in the urn:x-wiley:00027820:media:jace16832:jace16832-math-0010. For the local environment of Zr4+, the major form is ZrO7 with a trace of ZrO8.-
dc.languageeng-
dc.publisherWiley-Blackwell Publishing, Inc. The Journal's web site is located at http://onlinelibrary.wiley.com/journal/10.1111/(ISSN)1551-2916-
dc.relation.ispartofJournal of the American Ceramic Society-
dc.rightsSubmitted (preprint) Version This is the pre-peer reviewed version of the following article: [FULL CITE], which has been published in final form at [Link to final article using the DOI]. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. Accepted (peer-reviewed) Version This is the peer reviewed version of the following article: [FULL CITE], which has been published in final form at [Link to final article using the DOI]. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.-
dc.subjectnuclear waste-
dc.subjectphase transformations-
dc.subjectx-ray methods-
dc.subjectzirconolite-2M-
dc.titleSynchrotron X-ray Spectroscopy Investigation of the Ca1-xLnxZrTi2-x(Al,Fe)xO7 Zirconolite Ceramics (Ln=La, Nd, Gd, Ho, Yb)-
dc.typeArticle-
dc.identifier.emailLiao, C: liaocz@hku.hk-
dc.identifier.emailShih, K: kshih@hku.hk-
dc.identifier.authorityShih, K=rp00167-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1111/jace.16832-
dc.identifier.scopuseid_2-s2.0-85074265321-
dc.identifier.hkuros318654-
dc.identifier.volume103-
dc.identifier.issue2-
dc.identifier.spage1463-
dc.identifier.epage1475-
dc.identifier.isiWOS:000490398400001-
dc.publisher.placeUnited States-
dc.identifier.issnl0002-7820-

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