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Author |
Sun, J.; Chen, Q.; Qin, W.; Wu, H.; Liu, B.; Li, S.; Bogaerts, A. |
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Title |
Plasma-catalytic dry reforming of CH4: Effects of plasma-generated species on the surface chemistry |
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A1 Journal Article |
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Year  |
2024 |
Publication |
Chemical Engineering Journal |
Abbreviated Journal |
Chemical Engineering Journal |
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Volume |
498 |
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Pages |
155847 |
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Keywords |
A1 Journal Article; Dry reforming of methane Plasma catalysis Plasma-enhanced surface chemistry Path flux and sensitivity analysis Coking kinetics; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ; |
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Abstract |
By means of steady-state experiments and a global model, we studied the effects of plasma-generated reactive species on the surface chemistry and coking in plasma-catalytic CH4/CO2 reforming at reduced pressure (8–40 kPa). We used a hybrid ZDPlasKin-CHEMKIN model to predict the species densities over time. The detailed plasma-catalytic mechanism consists of the plasma discharge scheme, a gas-phase chemistry set and a surface mechanism. Our experimental results show that the coupling of Ni/SiO2 catalyst with plasma is more effective in CH4/CO2 activation and conversion than unpacked DBD plasma, with syngas being the main products. The
highest total conversion of 16 % was achieved at 8000 V and 473 K, with corresponding CO and H2 yields of 15 % and 12 %, respectively. The reactants conversion and product selectivity are well captured by the kinetic model. Our simulation results suggest that vibrational species and radicals can accelerate the dissociative adsorption and Eley-Rideal (E-R) reactions. Path flux analysis shows that E-R reactions dominate the surface reaction pathways, which differs from thermal catalysis, indicating that the coupling of non-equilibrium plasma and catalysis can effectively shift the formation and consumption pathways of important adsorbates. For instance, our model suggests that HCOO(s) is primarily generated through the E-R reaction CO2(v) + H(s) → HCOO(s), while the hydrogenation reaction HCOO(s) + H → HCOOH(s) is the main source of HCOOH(s). Carbon deposition on the
catalyst surface is primarily formed through the stepwise dehydrogenation of CH4, while the E-R reactions enhanced by plasma-generated H and O atoms dominate the consumption of carbon deposition. This work provides new insights into the effects of reactive species on the surface chemistry in plasma-catalytic CH4/CO2 reforming. |
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Publication Date |
2024-09-17 |
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ISSN |
1385-8947 |
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Impact Factor |
15.1 |
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Open Access |
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Notes |
National Natural Science Foundation of China; |
Approved |
Most recent IF: 15.1; 2024 IF: 6.216 |
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Call Number |
PLASMANT @ plasmant @ |
Serial |
9266 |
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