A melt-based reaction pathway for CO2 and CH4 conversion to syngas and carbon using liquid In–Sn
Bibliographic record
Abstract
• 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.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot 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.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.003 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
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".