A Structural and Spectroscopic Investigation of Hydrous and Anhydrous Rare-Earth Phosphates
Bibliographic record
Abstract
Nuclear power plants provide clean energy for generating electricity via neutron induced fission reactions of nuclear fuels and at the end of this energy generation process, radioactive waste is produced.Currently, the waste is chemically incorporated into a glass matrix and the resulting wasteform is destined for storage in geological repositories.Glass based wasteforms, however, might corrode under repository conditions and could potentially release radionuclides to the biosphere.Hence, crystalline wasteforms were proposed as an alternative to glass based wasteforms and among the many materials studied, materials adopting the monazite-(REPO 4 ; RE = La to Gd) and xenotime-(RE'PO 4 ; RE' = Tb to Lu and Y) type structures were suggested as a potential wasteform.Both monazite and xenotime are naturally abundant rare-earth minerals containing significant amounts of U and Th and have remained stable on a geological time-scale.Hydrous rare-earth phosphates adopting the rhabdophane-type structure (REPO 4 .nH 2 O; RE = La to Dy) also exist in nature and are present on the surface of anhydrous rare-earth minerals (e.g., monazite).The hydrous phase may act as a secondary barrier by preventing the release of actinides from reaching the biosphere.This thesis aims to provide an atomic level understanding of hydrous and anhydrous rare-earth phosphates using X-ray based diffraction and spectroscopic techniques.A comprehensive account of the rich structural chemistry of rare-earth phosphates are provided in Chapters 2 and 3 using X-ray diffraction (XRD) and X-ray absorption near-edge spectroscopy (XANES).Crystalline materials containing radioactive wastes are prone to undergo radiation-induced structural damage and, in Chapter 4, radiation damage studies on monaziteand xenotime-type materials were conducted by simulating radiation damage events using highenergy ion implantation.The results from this study depict the ability of these materials to recover from the structural damage inflicted by high energy ion-implantation.In Chapter 5, the chemical durability of rare-earth phosphates was studied by investigating leaching behaviour of these materials in deionized water.Preliminary results suggest a faster leaching of hydrous rareearth phosphates when compared to their anhydrous counterparts.The information presented in this thesis will contribute to the growing body of work on crystalline wasteforms for nuclear waste immobilization.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".