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Record W2971373933 · doi:10.1021/acscatal.9b03301

Understanding Acidity of Molten Salt Hydrate Media for Cellulose Hydrolysis by Combining Kinetic Studies, Electrolyte Solution Modeling, Molecular Dynamics Simulations, and <sup>13</sup>C NMR Experiments

2019· article· en· W2971373933 on OpenAlexafffund
Natalia Rodriguez Quiroz, Arul Mozhi Devan Padmanathan, Samir H. Mushrif, Dionisios G. Vlachos

Bibliographic record

VenueACS Catalysis · 2019
Typearticle
Languageen
FieldEngineering
TopicBiofuel production and bioconversion
Canadian institutionsUniversity of Alberta
FundersBasic Energy SciencesNatural Sciences and Engineering Research Council of CanadaUniversity of Alberta
KeywordsChemistryCellobioseHydrolysisDissolutionInorganic chemistryHydrateSalt (chemistry)CelluloseMolecular dynamicsSolvationCellulaseDepolymerizationMoleculeOrganic chemistryComputational chemistry

Abstract

fetched live from OpenAlex

Depolymerization of lignocellulosic biomass in concentrated metal salts and more specifically in acidified LiBr molten salt hydrate (AMSH) results in high glucose yields at low acid concentrations, low temperatures, and very short times with potentially considerable economic benefits. However, our understanding of this promising medium is limited. Here, we study the effect of different LiBr concentrations on acidity and hydrolysis of cellobiose, a cellulose surrogate molecule, in dilute H2SO4 solutions. We use thermodynamic modeling to predict the H+(hydron) activity and the speciation and correlate these with the experimentally measured reaction rates. We find that the main contribution of the salt to the reactivity stems from the dramatic increase in H+ activity and secondary to an interaction of salt with the acid species that effectively renders the inorganic acid very strong. We perform molecular dynamics simulations and reveal that the increased hydron activity can be attributed to the decrease in the number of water molecules in the hydron solvation shell upon salt addition. Additionally, we extend the analysis to other salts and acids, concluding that the effects of different cations, anions, and acids in cellobiose hydrolysis likewise can be attributed to primarily changes in acidity. A key physicochemical descriptor of various salts is their enthalpy of dissolution. Finally, we explore the use of 13C NMR spectroscopy to estimate the pH of AMSH solutions.

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 categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Simulation or modeling · Consensus signal: Simulation or modeling
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.218
Threshold uncertainty score0.942

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 head0.032
GPT teacher head0.240
Teacher spread0.209 · 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.

The models applied no category: nothing in the taxonomy fit this work.
Study designSimulation or modeling
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

Citations63
Published2019
Admission routes2
Has abstractyes

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