Emerging disorder in Gd2(Ti1−xZrx)2O7 pyrochlores matrices for radioactive waste disposal: symmetry lowering versus defect clustering

Literature Information

Publication Date 2023-10-26
DOI 10.1039/D3TA04847K
Impact Factor 12.732
Authors

Armando di Biase, Carlo Castellano, Giorgia Confalonieri, Patrizia Fumagalli, Simone Tumiati, Davide Ceresoli


View Original

Abstract

Pyrochlore compositions in the Gd2(Ti1−xZrx)2O7 solid solution have gained attention in the field of radioactive waste forms because they are capable of withstanding high doses of ion irradiation without becoming amorphous, as the Zr-content increases. The purpose of this study was to explore the structure of Gd2(Ti1−xZrx)2O7 compounds at various length scales using Synchrotron High-Resolution X-ray Powder Diffraction (HR-XRPD), Pair Distribution Function (PDF) analysis, and Raman spectroscopy. Through Rietveld analysis of HR-XRPD patterns, it was determined that substituting Ti with Zr in the Gd2Ti2O7 compound results in the gradual formation of Anti-Frenkel (AFr) Oxygen defects and, for xZr ≥ 0.75, in slight cation A/B site disordering, while still maintaining the same average pyrochlore structure. Raman spectroscopy shows a marked change in the spectra for xZr ≥ 0.50, with a general broadening of the bands and the emergence of new spectral features, indicating an increase in static disorder and some symmetry breaks at shorter length scales. This outcome was confirmed by PDF modelling in the low r region. Two alternative models were proposed to map the disorder: (i) a Pmma weberite-type structure, which suitable fits the PDFs in the Zr-rich part of the phase diagram only up to r ≈ 8 Å; (ii) a disordered pyrochlore structure containing Anti-Frenkel (AFr) pairs in the form of extended clusters as generated by DFT calculations. The short r range of applicability of the weberite-type model and the computed energy values tip the balance in favor of the AFr clusters.

Related Literature

Dense arrangement of crown ethers in graphene: novel graphitic carbon oxides with enhanced optoelectronic properties

Hongyan Li, Jiang Xiang, Jing Xu, Wei Liu

2023-12-12 Paper

DOI: 10.1039/D3CP03902A

Study on a direct hydrazine borane fuel cell based on an anion exchange membrane

Yang Zhang, Wenxing Jiang, Zhenying Chen, Yingying Liu, Chengwei Deng, Xiaodong Zhuang, Junliang Zhang, Changchun Ke

2023-11-30 Paper

DOI: 10.1039/D3SE01401K

Solar-driven electrochemical NH3 splitting into H2 and N2 on BiVO4-based photoanodes

Miwako Teranishi, Shin-ichi Naya, Hiroaki Tada

2023-12-13 Paper

DOI: 10.1039/D3SE01513K

Heat-transfer enhancement and optimization design of a roadway with typical angles using field synergy theory

Yongliang Zhang, Xilong Zhang, Mingjie Li, Yunfei Liu, Zhen Hu

2023-11-21 Paper

DOI: 10.1039/D3SE00989K

Inside front cover

2024-01-30 Cover

DOI: 10.1039/D4SE90010C

Unravelling the band splitting origin in bulk and 2D distorted α-CsPbI3 perovskite

Safieh Nazari, Fatemeh Mohammad Dezashibi, Nadia Babaei Bidmeshki

2023-12-05 Paper

DOI: 10.1039/D3CP04558G

Steam reforming of methane by titanium oxide photocatalysts with hollow spheres

Akira Yamaguchi, Tomoki Kujirai, Takeshi Fujita, Hideki Abe, Masahiro Miyauchi

2024-01-08 Paper

DOI: 10.1039/D3SE01346D

Understanding the “Berg limit”: the 65° contact angle as the universal adhesion threshold of biomatter

Matej Kanduč, Emanuel Schneck, Roland R. Netz

2023-12-12 Perspective

DOI: 10.1039/D3CP05084J

You might also like

Compound Q&A

How should waste containing N-Methoxy-N-methyl-1,3-thiazole-5-carboxamide (CAS: 898825-89-3) be handled?

Waste containing N-Methoxy-N-methyl-1,3-thiazole-5-carboxamide (CAS: 898825-89-3...

898825-89-3N-Methoxy-N-methyl-1...
Compound Q&A

How should N-(4-Biphenylyl)dibenzo[b,d]furan-4-amine (CAS: 1318338-47-4) be stored?

N-(4-Biphenylyl)dibenzo[b,d]furan-4-amine should be stored in a tightly sealed c...

1318338-47-4N-(4-Biphenylyl)dibe...
Compound Q&A

What is the market or research trend for 3-Acetamido-5-amino-2,4,6-triiodobenzoic acid (CAS: 1713-07-1)?

The market for 3-Acetamido-5-amino-2,4,6-triiodobenzoic acid (CAS: 1713-07-1) is...

1713-07-13-Acetamido-5-amino-...
Compound Q&A

How should Benzyl 2-O-acetyl-3,4,6-tri-O-benzyl-beta-D-galactopyranoside (CAS: 61820-03-9) be stored?

Benzyl 2-O-acetyl-3,4,6-tri-O-benzyl-beta-D-galactopyranoside (CAS: 61820-03-9) ...

61820-03-9Benzyl 2-O-acetyl-3,...
Compound Q&A

What regulatory guidelines apply to 2-Ethylpiperazine dihydrochloride (CAS: 438050-52-3)?

2-Ethylpiperazine dihydrochloride (CAS: 438050-52-3) is regulated under the Glob...

438050-52-32-Ethylpiperazine di...
Compound Q&A

What regulatory guidelines apply to 1,1'-[1,3-Phenylenebis(methylene)]bis(3-methyl-1H-pyrrole-2,5-dione) (CAS: 119462-56-5)?

1,1'-[1,3-Phenylenebis(methylene)]bis(3-methyl-1H-pyrrole-2,5-dione) (CAS: 11946...

119462-56-51,1'-[1,3-Phenyleneb...
Compound Q&A

Are there alternatives to 5-Fluoro-2-(1-pyrrolidinyl)pyridine (CAS: 1287217-79-1) in synthesis?

Several alternatives can be used in the synthesis of 5-Fluoro-2-(1-pyrrolidinyl)...

1287217-79-15-Fluoro-2-(1-pyrrol...
Compound Q&A

What precautions should be taken when handling 6-Bromoimidazo[1,2-a]pyridin-8-amine (CAS: 676371-00-9)?

When handling 6-Bromoimidazo[1,2-a]pyridin-8-amine, it is important to wear appr...

676371-00-96-Bromoimidazo[1,2-a...
Compound Q&A

Are there alternatives to (2S,4R)-4-(4-Nitrobenzyl)pyrrolidine-2-carboxylic acid hydrochloride (CAS: 1049740-22-8) in synthesis?

Alternatives to (2S,4R)-4-(4-Nitrobenzyl)pyrrolidine-2-carboxylic acid hydrochlo...

1049740-22-8(2S,4R)-4-(4-Nitrobe...

Source Journal

Journal of Materials Chemistry A

Journal of Materials Chemistry A
CiteScore: 19.5
Self-citation Rate: 4.7%
Articles per Year: 2211

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment

Recommended Compounds

Recommended Suppliers

Disclaimer
This page provides academic journal information for reference and research purposes only. We are not affiliated with any journal publishers and do not handle publication submissions. For publication-related inquiries, please contact the respective journal publishers directly.
If you notice any inaccuracies in the information displayed, please contact us at support@chemtradehub.com. We will promptly review and address your concerns.