Abstract
A newly established stagnation flow reactor with analysis of spatially resolved concentrations profiles is presented as useful tool for the investigation of heterogeneously catalyzed gas-phase reactions. The simplicity of this laboratory-scale reactor enables detailed modeling of the diffusive and convective transport within the one-dimensional gas-phase boundary-layer coupled with elementary-step homogeneous and heterogeneous reaction mechanisms. This set-up is applied to study the kinetics of hydrogen oxidation over Rh/Al2O3. By combining experimental and modeling results for a wide range of temperature and fuel/oxygen ratios, a thermodynamically consistent set of kinetic data for a 12-step surface reaction mechanism is derived. The applicability of the mechanism is further tested by the model prediction of experimentally derived ignition temperatures in a stagnation flow reactor and oxygen conversion in H2-rich hydrogen oxidation in an annular flow reactor at varying flow rate and temperature.
| Original language | English |
|---|---|
| Pages (from-to) | 171-184 |
| Number of pages | 14 |
| Journal | Chemical Engineering Science |
| Volume | 89 |
| DOIs | |
| State | Published - Feb 5 2013 |
| Externally published | Yes |
Funding
This work was supported by Deutsche Forschungsgemeinschaft (DFG) . We gratefully acknowledge R.J. Kee, N.P. Sullivan, and N.E. McGuire (all Colorado School of Mines) for a fruitful collaboration in the reactor development. We also thank S. Tischer and H. Karadeniz (both KIT) for their support using DETCHEM. We acknowledge B. Reznik (KIT) for LEM and SEM studies and Julian N. Bär (KIT) for his help on the simulation of the catalytic ignition experiments.
| Funders | Funder number |
|---|---|
| Deutsche Forschungsgemeinschaft |
Keywords
- Heterogeneous catalysis
- Hydrogen oxidation
- Kinetics
- Modeling
- Rhodium
- Stagnation-flow reactor