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Record W2624730306

Cerium Oxidation State in Silicate Melts and the Application to Ce-in-Zircon Oxygen Barometry

2013· dissertation· en· W2624730306 on OpenAlexfundaboutno aff
Duane J. Smythe

Bibliographic record

VenueTSpace (University of Toronto) · 2013
Typedissertation
Languageen
FieldEconomics, Econometrics and Finance
TopicGeochemistry and Geochronology of Asian Mineral Deposits
Canadian institutionsnot available
FundersGovernment of OntarioUniversity of TorontoGeological Society of America
KeywordsZirconSilicateCeriumGeochemistryOxidation stateOxygenMineralogyGeologyMaterials scienceChemistryMetallurgy
DOInot available

Abstract

fetched live from OpenAlex

Through measurements of cerium redox equilibrium in silicate melts, and an internally-consistent model for zircon-melt partitioning of Ce, a calibration for estimating the redox conditions during zircon crystallization is presented. To quantify Ce4+/Ce3+ in natural magmas, Ce doped silicate glasses ranging in composition from basalt to rhyolite (± H2O) at 0.001 and 1 GPa, under fO2 conditions varying from FMQ –6.0 to +8.4 (where FMQ is the fayalite-magnetite-quartz oxygen buffer), and temperatures from 1200 to 1500°C were synthesized. 
\nSamples were analyzed using both synchrotron-based Ce M4,5-edge x-ray absorption near edge structure (XANES) spectroscopy and traditional wet chemical techniques. Based on comparison to potentiometric determinations of Ce4+/Ce3+ in digested portions of our samples, Ce4+ was found to have a greater fluorescence yield (FLY) response to the incident radiation in the M4,5-edge XANES region than Ce3+. A correction to M-edge determined Ce4+/Ce3+ ratios as follows: 
\nCe4+/Cetotal=587.7[Ce4+/Cetotal+/-5%]XANES^A(+/-0.004) (0<Ce4+/Cetotal<0.4)
\nwhere the exponent A is a function of the number of non-bridging oxygens per tetrahedrally-coordinated cation (NBO/T) for a given glass composition, [Ce4+/Cetotal]XANES is the contribution from Ce4+ to the M4,5-edge area over the total area of the M4,5-edge, and Ce4+/Cetotal is the actual fraction of Ce4+ in the sample. 
\nFor a given melt composition, the change in Ce4+/Ce3+ with fO2 follows the thermodynamically predicted trend assuming simple oxides as melt species. In addition to fO2, melt composition and water content have been found to be secondary controls on Ce4+/Ce3+, with more depolymerized melts and hydrous compositions favoring the stabilization of Ce3+. The Ce4+/Ce3+ ratio can be expressed through the equation,
\nlog(Ce4+/Ce3+)=1/4logfO2+5705(+/-257)/T-0.8694(+/-0.005)NBO/T-3.856(+/-0.049)xH2O-3.889(+/-0.102)
\nwhere T is in Kelvin, and xH2O is the mole fraction of water in the melt. 
\nUsing this model, fO2 for samples from the Bishop tuff (USA), Toba tuff (Indonesia) and Nain plutonic suite (Canada), have been calculated and are in excellent agreement (typically within 0.5 log units) with independent estimates. Using the composition of the Jack Hills Hadean zircons, combined with estimates of parental magma composition, the fO2 during zircon crystallization was determined to be between FMQ -1.0 to +2.5, suggesting that relatively oxidized magmatic source regions, similar to 3.5 Ga komatiite suites, existed by ~4.4 Ga.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not 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.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesInsufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Observational · Consensus signal: none
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.943
Threshold uncertainty score0.999

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0020.000

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.

Opus teacher head0.007
GPT teacher head0.199
Teacher spread0.192 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designObservational
Domainnot available
GenreEmpirical

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".

Quick stats

Citations2
Published2013
Admission routes2
Has abstractyes

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