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Record W4387119035 · doi:10.1021/acs.chemmater.3c01777

Unlocking the Separation Capacities of a 3D-Iron-Based Metal Organic Framework Built from Scarce Fe<sub>4</sub>O<sub>2</sub> Core for Upgrading Natural Gas

2023· article· en· W4387119035 on OpenAlexafffund
Himan Dev Singh, Piyush Singh, Raviraju Vysyaraju, Bhubesh Murugappan Balasubramaniam, Deepak Rase, Pragalbh Shekhar, Arvind Rajendran, Ramanathan Vaidhyanathan

Bibliographic record

VenueChemistry of Materials · 2023
Typearticle
Languageen
FieldChemistry
TopicMetal-Organic Frameworks: Synthesis and Applications
Canadian institutionsUniversity of Alberta
FundersAir Force Office of Scientific ResearchScience and Engineering Research BoardMinistry of Education, IndiaNatural Sciences and Engineering Research Council of CanadaIndian Institute of Science Education and Research PuneCouncil of Scientific and Industrial Research, IndiaDepartment of Science and Technology, Ministry of Science and Technology, India
KeywordsSelectivityAdsorptionMetal-organic frameworkMoietyMethaneSorbentAmine gas treatingChemical engineeringChemistryCarboxylateNatural gasBar (unit)Langmuir adsorption modelMaterials scienceInorganic chemistryOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

Methane is an important alternative fuel, and upgrading it to improve fuel efficiency is an imperative target. Solid sorbents capable of selectively removing the major impurities CO 2 and N 2 from the natural gas contribute immensely to this process. We report a porous 3D iron-MOF built by linking scarce Fe 4 O 18 N 2 clusters through readily available terephthalate and diaminotrizaole ligands. The 1-D channels with a high density of polarizing amine groups, aromatic rings, and carboxylate oxygen adsorb CO 2 and the even less polarizable CH 4 . The MOF uptakes 4.7 mmol/g of CO 2 at 273 K, 1 bar, with an optimal heat of adsorption of ≈24.5 kJ/mol and CO 2 /N 2 IAST selectivity of ≈26. At higher pressures, the MOF exhibits a Langmuir type isotherm for methane and nitrogen with a CH 4 /N 2 IAST selectivity of ≈4. The MOF’s excellent cyclic stability is affirmed by the TGA- and iso-cycling. Modeling studies propound the amine’s interactions with the CO 2, but more dominant is the CO 2 ···CO 2 cooperative interactions. At 20 bar, CH 4 interacts with many framework sites through weak dispersive interactions. In contrast, N 2 interacts specifically with the triazole moiety; thus, the MOF favors the former. The CO 2, CH 4, and N 2 diffusion coefficients, calculated using MD simulations, are quite favorable (Dc for CO 2 = 1.11 × 10 –6; CH 4 = 9.04 × 10 –6; N 2 = 1.875 × 10 –5 cm 2 /s). The dynamic breakthrough studies confirm the potential of the Fe-MOF to separate the gas mixtures. With these advantageous sorbent characteristics of this Fe-MOF, we propose using it in a two-stage PSA for the natural gas purification process, Stage I: removal of CO 2 and Stage II: removal of N 2 . The outcomes point to the potential of a readily accessible iron-based amine MOF as sorbent for natural gas upgrading. A process optimization using a 4-step PSA validates the ability of our MOF to yield >96% purity of CH 4 as required for pipeline transportation.

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 machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation 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 score0.001
Threshold uncertainty score0.002

Distilled classifier scores by category (both heads)

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)0.0010.000

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 head0.024
GPT teacher head0.261
Teacher spread0.237 · 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 source (direct Gemma or distilled Codex), 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

Citations9
Published2023
Admission routes2
Has abstractyes

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