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Characterization of Acid-Soluble Oxidized Asphaltenes by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry: Insights on Oxycracking Processes and Asphaltene Structural Features

2015· article· en· W2290194895 on OpenAlexfundno aff
Renzo C. Silva, Jagoš R. Radović, Farouq Ahmed, Ursula Ehrmann, Melisa Brown, Lante Carbognani Ortega, Steve Larter, Pedro Pereira‐Almao, Thomas B. P. Oldenburg

Bibliographic record

VenueEnergy & Fuels · 2015
Typearticle
Languageen
FieldChemistry
TopicPetroleum Processing and Analysis
Canadian institutionsnot available
FundersNatural Sciences and Engineering Research Council of CanadaCanada Research ChairsCanada Foundation for InnovationUniversity of Calgary
KeywordsFourier transform ion cyclotron resonanceAsphalteneChemistryMass spectrometryAnalytical Chemistry (journal)Organic chemistryChromatography

Abstract

fetched live from OpenAlex

The dissolution of organic matter into water via oxidative processes, named oxycracking, has been practiced for a long time for the removal of organic pollutants, in which oxygen induces breakage and functionalization of organic molecules. Recently, oxycracking has been explored as an alternative approach to handling the increased amount of solid residues produced in oil sands upgrading activities that involve carbon rejection in solvent deasphalting units. This study uses an asphaltene-rich feedstock, operationally known as petroleum pitch, isolated from an Athabasca bitumen vacuum residue, which was submitted to oxycracking reactions at 200 and 220 °C. The feed and water-soluble fractions isolated at pH 1, termed acid-soluble oxidized asphaltenes (ASOA), were analyzed by ultrahigh-resolution mass spectrometry [Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS)] using electrospray and atmospheric pressure photoionization ion sources. FTICR-MS analysis revealed extensive oxidation of all compound classes originally present in the asphaltene-rich feed. Double bond equivalent (DBE) distribution plots show that sequential carboxylation (formation of a carboxyl group) occurs progressively with an increasing reaction temperature, leading to the incorporation of up to 15 oxygen atoms per molecule, whereas simultaneous decarboxylation reactions produce a CO 2 -rich gas phase. ASOA samples also show lower overall carbon number distributions than the asphaltene feed, which is direct evidence of C–C bond cleavage during the oxycracking process. In addition, molecular fragments detected in ASOA after carbon–carbon bond cleavages showed not only lower carbon numbers but also lower DBEs per molecule, consistent with a more dominant archipelago architecture for the parent asphaltene molecules.

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 categoriesMeta-epidemiology (narrow)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.014
Threshold uncertainty score1.000

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)0.0000.000

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 head0.009
GPT teacher head0.225
Teacher spread0.215 · 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 designBench or experimental
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

Citations25
Published2015
Admission routes1
Has abstractyes

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