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| Main Authors: | , |
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| Format: | Preprint |
| Published: |
2025
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2508.02214 |
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| _version_ | 1866916879409348608 |
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| author | Ritov, Esther Dana, Alon Grinberg |
| author_facet | Ritov, Esther Dana, Alon Grinberg |
| contents | Dry reforming of methane (DRM) over platinum catalysts offers a promising route for CO2 utilization and syngas (H2/CO) production, a versatile feedstock for synthetic fuels. This study employs automated chemical kinetic model generation to present a detailed microkinetic mechanism for Pt-catalyzed DRM between 700-1100 K, identifying key reaction pathways and kinetic limitations through sensitivity analysis.
Model predictions of CH4 and CO2 conversion and syngas production closely match fixed-bed experimental data across the entire temperature range and varied feed ratios. Our predictive reaction network reveals that OCX serves as a critical bottleneck intermediate for cooperative CH4 and CO2 activation. While CO desorption (OCX <=> CO + X) was identified as the most influential step with strong negative sensitivity toward methane concentration, OCX regeneration (CO2X + CX <=> 2OCX) inhibits methane conversion by maintaining surface saturation.
Methane activation follows sequential C-H scissions (CH4X -> CH3X -> CH2X -> CHX -> CX), while CO2 activation proceeds predominantly via a hydrogen-mediated carboxyl route (CO2X + HX -> COOHX -> COX + OHX). Three operational regimes were identified: low-temperature desorption-limited kinetics (700-850 K), transitional pathway activation (850-950 K), and high-temperature distributed control with carbon management challenges (950-1300 K).
These insights provide design principles for platinum-based DRM catalysts, emphasizing temperature-specific optimization strategies. This is the first study to apply fully automated microkinetic model generation to Pt-catalyzed DRM, integrating sensitivity analysis, flux analysis, and surface speciation for catalyst design. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2508_02214 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Predictive Chemical Kinetic Modeling of Pt-Catalyzed Dry Methane Reforming Ritov, Esther Dana, Alon Grinberg Computational Physics Dry reforming of methane (DRM) over platinum catalysts offers a promising route for CO2 utilization and syngas (H2/CO) production, a versatile feedstock for synthetic fuels. This study employs automated chemical kinetic model generation to present a detailed microkinetic mechanism for Pt-catalyzed DRM between 700-1100 K, identifying key reaction pathways and kinetic limitations through sensitivity analysis. Model predictions of CH4 and CO2 conversion and syngas production closely match fixed-bed experimental data across the entire temperature range and varied feed ratios. Our predictive reaction network reveals that OCX serves as a critical bottleneck intermediate for cooperative CH4 and CO2 activation. While CO desorption (OCX <=> CO + X) was identified as the most influential step with strong negative sensitivity toward methane concentration, OCX regeneration (CO2X + CX <=> 2OCX) inhibits methane conversion by maintaining surface saturation. Methane activation follows sequential C-H scissions (CH4X -> CH3X -> CH2X -> CHX -> CX), while CO2 activation proceeds predominantly via a hydrogen-mediated carboxyl route (CO2X + HX -> COOHX -> COX + OHX). Three operational regimes were identified: low-temperature desorption-limited kinetics (700-850 K), transitional pathway activation (850-950 K), and high-temperature distributed control with carbon management challenges (950-1300 K). These insights provide design principles for platinum-based DRM catalysts, emphasizing temperature-specific optimization strategies. This is the first study to apply fully automated microkinetic model generation to Pt-catalyzed DRM, integrating sensitivity analysis, flux analysis, and surface speciation for catalyst design. |
| title | Predictive Chemical Kinetic Modeling of Pt-Catalyzed Dry Methane Reforming |
| topic | Computational Physics |
| url | https://arxiv.org/abs/2508.02214 |