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Record W2991304157 · doi:10.1021/jacs.9b10251

Controlling the Polymorphism and Topology Transformation in Porphyrinic Zirconium Metal–Organic Frameworks via Mechanochemistry

2019· article· en· W2991304157 on OpenAlexafffund
Bahar Karadeniz, Dijana Žilić, Igor Huskić, Luzia S. Germann, Athena M. Fidelli, Senada Muratović, Ivor Lončarić, Martin Etter, Robert E. Dinnebier, Dajana Barišić, Nikola Cindro, Timur İslamoğlu, Omar K. Farha, Tomislav Friščić, Krunoslav Užarević

Bibliographic record

VenueJournal of the American Chemical Society · 2019
Typearticle
Languageen
FieldChemistry
TopicMetal-Organic Frameworks: Synthesis and Applications
Canadian institutionsMcGill University
FundersEuropean Social FundDefense Threat Reduction AgencyNatural Sciences and Engineering Research Council of CanadaHrvatska Zaklada za ZnanostEuropean Cooperation in Science and Technology
KeywordsMechanochemistryZirconiumMetal-organic frameworkChemistryElectron paramagnetic resonancePorphyrinSynchrotronTopology (electrical circuits)Polymorphism (computer science)CrystallographyAdsorptionInorganic chemistryPhotochemistryOrganic chemistryNuclear magnetic resonance

Abstract

fetched live from OpenAlex

Tetratopic porphyrin-based metal–organic frameworks (MOFs) represent a particularly interesting subclass of zirconium MOFs due to the occurrence of several divergent topologies. Control over the target topology is a demanding task, and reports often show products containing phase contamination. We demonstrate how mechanochemistry can be exploited for controlling the polymorphism in 12-coordinated porphyrinic zirconium MOFs, obtaining pure hexagonal PCN-223 and cubic MOF-525 phases in 20–60 min of milling. The reactions are mainly governed by the milling additives and the zirconium precursor. In situ monitoring by synchrotron powder X-ray diffraction revealed that specific reaction conditions resulted in the formation of MOF-525 as an intermediate, which rapidly converted to PCN-223 upon milling. Electron spin resonance measurements revealed significant differences between the spectra of paramagnetic centers in two polymorphs, showing a potential of polymorphic Zr-MOFs as tunable supports in spintronics applications.

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: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.011
Threshold uncertainty score0.707

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.002
Insufficient payload (model declined to judge)0.0010.000

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 head0.006
GPT teacher head0.224
Teacher spread0.218 · 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 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

Citations115
Published2019
Admission routes2
Has abstractyes

Explore more

Same venueJournal of the American Chemical SocietySame topicMetal-Organic Frameworks: Synthesis and ApplicationsFrench-language works237,207