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Record W4414837463 · doi:10.1016/j.jcat.2025.116465

A melt-based reaction pathway for CO2 and CH4 conversion to syngas and carbon using liquid In–Sn

2025· article· en· W4414837463 on OpenAlex
Genpei Cai, Nikil Surya RajaPrabu, J. B. Srivastava, Korbinian Lechner, Jorit Körber, Zhiyuan Zong, Kevin J. Smith, Vishal Agarwal, D. Chester Upham

Why this work is in the frame

A frame that forgets how it found something cannot be audited. These are the routes that admitted this work.

affAt least one author lists a Canadian institution in the pinned OpenAlex snapshot.
fundA Canadian funder is recorded on the work.

Bibliographic record

VenueJournal of Catalysis · 2025
Typearticle
Languageen
FieldChemical Engineering
TopicCatalysts for Methane Reforming
Canadian institutionsUniversity of British Columbia
FundersScience and Engineering Research BoardAlliance de recherche numérique du CanadaNatural Sciences and Engineering Research Council of CanadaMinistry of Education, IndiaUniversity of British ColumbiaIndian Institute of Technology KanpurDepartment of Science and Technology, Ministry of Science and Technology, IndiaCanada Foundation for Innovation
KeywordsSyngasCatalysisMethaneCarbon fibersPyrolysisActivation energyDensity functional theoryMolecular dynamics

Abstract

fetched live from OpenAlex

• Molten In–Sn catalyzes CH 4 pyrolysis and dry reforming to produce syngas and solid carbon. • Reaction proceeds via unique solvated [C] and [O] intermediates in a molten metal catalyst. • DFT and experiments reveal CH 4 and CO 2 activation barriers in molten In–Sn. • Accumulated carbon lowers CO 2 activation energy, enhancing catalytic performance. • Dynamic surface properties enable efficient CO 2 and CH 4 conversion at high temperatures. Molten In–Sn has been recently reported as an effective catalyst for directly producing 2:1 H 2 :CO syngas and solid carbon from CO 2 and CH 4 in a single reaction, equivalent to the combined reactions of methane pyrolysis and dry reforming. In the present work, when reactants are alternately fed, mass balances indicate that CO 2 reacts to form an [O] species that oxidizes CH 4 . Also, CH 4 is converted to a [C] species that reduces CO 2 . The presence of accumulated [O] did not significantly affect the experimentally determined activation energies of 229 kJ/mol vs. 222 kJ/mol. We performed ab initio molecular dynamics (AIMD) simulations and density functional theory (DFT) calculations, to probe the dynamic structural evolution and to obtain atomistic insights into the behavior of the molten In–Sn alloy at the molecular level. This integrated approach also facilitated the evaluation of activation energy barriers associated with key reaction pathways. Simulations indicate that [O] are solvated; rapidly switching neighbors between Sn and In, which is unique to a molten catalyst. The presence of accumulated [C] significantly decreased the experimentally observed apparent CO 2 activation energy from 154 kJ/mol to 75 kJ/mol, which is lower than the direct reaction between CO 2 and solid graphite. This finding supports the simulations that indicate [C] formed in the melt is solvated, chemically distinct from solid carbon, and can play a critical role in enhancing catalytic performance. Large fluctuations in adsorbate binding energies were theoretically observed over time, suggesting the creation of transient sites that are fleetingly active, and facilitate the formation of solvated [O] and [C] intermediates unique to a molten catalyst surface.

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.

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 score0.023
Threshold uncertainty score0.407

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0010.000
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 head0.010
GPT teacher head0.258
Teacher spread0.247 · 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