A comparative experimental and numerical investigation of the heterogeneous and homogeneous combustion characteristics of fuel-rich methane mixtures over rhodium and platinum

Sui, Ran; Mantzaras, John; Bombach, Rolf

doi:10.1016/j.proci.2016.06.001

Cited by 31 publications

(33 citation statements)

References 20 publications

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“…36 The development Figure 1: A diagram of the computational domain overlaid over the outline of the experimental configuration at the Paul Scherrer Institute. [42][43][44][45] of the mechanism was based on experimental data from the stagnation flow configuration of Karadeniz et al 37 Validation was also performed against experimental data covering the effect of inlet temperature on catalyst stability and outlet composition. 38,39 Recent DFT studies include detailed energetics of CO, C 2 and oxygenated compounds 40 and the impact of surface coordination on product selectivity on various Rh surfaces.…”

Section: Data Set Selectionmentioning

confidence: 99%

“…41 The experimental data sets selected for validation provide a consistent treatment for Pt and Rh catalysts and feature a subset of the conditions investigated using a high-pressure chamber. [42][43][44][45] The corresponding computational domain is shown in Fig. 1.…”

Section: Data Set Selectionmentioning

confidence: 99%

“…Calculated using the VTST mechanism for Rh with the gas phase chemistry of Lindstedt and Waldheim 55. Skevis 56 result in a large under-prediction of the ignition distance (< 30 mm downstream) and uncertainties in the gas phase chemistry are hence a major cause of discrepancies.The results for partial oxidation over Rh for case Rh1 of Sui et al45 are shown inFigs. 16 and 17.…”

mentioning

confidence: 99%

“…Experimental (symbols) and computational (lines) transverse mol fraction profiles for case Pt3 of Sui et al45 Symbols as inFig. 6.…”

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confidence: 99%

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Microkinetic Mechanisms for Partial Oxidation of Methane over Platinum and Rhodium

Kraus

Lindstedt

2017

J. Phys. Chem. C

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A systematic approach for the development of heterogeneous mechanisms is applied and evaluated for the catalytic partial oxidation of methane over platinum (Pt) and rhodium (Rh). The derived mechanisms are self-consistent and based on a reaction class-based framework comprising variational transition state theory (VTST) and two-dimensional collision theory for the calculation of pre-exponential factors with barrier heights obtained using the unity bond index-quadratic exponential potential (UBI-QEP) method. The surface chemistry is combined with a detailed chemistry for the gas phase and the accuracy of the approach is evaluated over Pt for a wide range of stoichiometries (0.3 ≤ φ ≤ 4.0), pressures (2 ≤ P (bar) ≤ 16) and residence times. It is shown that the derived mechanism can reproduce experimental data with an accuracy comparable to the prevalent collision theory approach and without the reliance on experimental data for sticking coefficients. The derived mechanism for Rh shows encouraging agreement for a similar set of conditions and the robustness of the approach is further evaluated by incorporating partial updates via more accurate DFT determined barrier heights. Substantial differences are noted for some channels (e.g. where reaction progress is strongly influenced by early transition states) though the impact on the overall agreement with experimental data is moderate for the current systems. Remaining discrepancies are explored using sensitivity analyses to establish key parameters. The study suggests that the overall framework is well-suited for the efficient generation of heterogeneous reaction mechanisms, that it can serve to identify key parameters where high accuracy ab initio methods are required and that it permits the inclusion of such updates as part of a gradual refinement process.

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Section: Data Set Selectionmentioning

confidence: 99%

Section: Data Set Selectionmentioning

confidence: 99%

mentioning

confidence: 99%

“…Experimental (symbols) and computational (lines) transverse mol fraction profiles for case Pt3 of Sui et al45 Symbols as inFig. 6.…”

mentioning

confidence: 99%

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Microkinetic Mechanisms for Partial Oxidation of Methane over Platinum and Rhodium

Kraus

Lindstedt

2017

J. Phys. Chem. C

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“…This technique represents a powerful method to gain detailed insight into the reactor during operation in a non-intrusive manner. Sui et al [24,25] studied the hetero-/homogeneous combustion of CH 4 /O 2 /N 2 mixtures over rhodium in this set up.The experiments included in situ spatially-resolved Raman measurements of gas phase species concentrations for evaluating the catalytic processes, and planar laser induced fluorescence (LIF) of the OH radical for assessing homogeneous combustion.…”

Section: Overview Of Experimental Setupsmentioning

confidence: 99%

CaRMeN: An Improved Computer-Aided Method for Developing Catalytic Reaction Mechanisms

et al. 2019

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The software tool CaRMeN (Catalytic Reaction Mechanism Network) was exemplarily used to analyze several surface reaction mechanisms for the combustion of H2, CO, and CH4 over Rh. This tool provides a way to archive and combine experimental and modeling information as well as computer simulations from a wide variety of sources. The tool facilitates rapid analysis of experiments, chemical models, and computer codes for reactor simulations, helping to support the development of chemical kinetic models and the analysis of experimental data. In a comparative study, experimental data from different reactor configurations (channel, annular, and stagnation flow reactors) were modeled and numerically simulated using four different catalytic reaction mechanisms from the literature. It is shown that the software greatly enhanced productivity.

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Spatially and Temporally Resolved Measurements of NO Adsorption/Desorption over NOx‐Storage Catalyst

et al. 2020

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The two‐dimensional (2D) temporal evolution of the NO‐concentration over a NOx‐storage catalyst is investigated in situ with planar laser‐induced fluorescence (PLIF) in an optically accessible parallel wall channel reactor. Signal accumulated phase‐correlated 2D‐recordings of repetitive adsorption/desorption cycles are obtained by synchronizing the switching of the NO gas flow (on/off) with the laser and detection system, thereby significantly increasing the signal‐to‐noise ratio. The gas compositions at the reactor outlet are additionally monitored by ex‐situ analytics. The impacts of varying feed concentration, temperature and flow velocities are investigated in an unsteady state. Transient kinetics and the mass transfer limitations can be interpreted in terms of the NO concentration gradient changes. The technique presented here is a very useful tool to investigate the interaction between surface kinetics and the surrounding gas flow, especially for transient catalytic processes.

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A comparative experimental and numerical investigation of the heterogeneous and homogeneous combustion characteristics of fuel-rich methane mixtures over rhodium and platinum

Cited by 31 publications

References 20 publications

Microkinetic Mechanisms for Partial Oxidation of Methane over Platinum and Rhodium

Microkinetic Mechanisms for Partial Oxidation of Methane over Platinum and Rhodium

CaRMeN: An Improved Computer-Aided Method for Developing Catalytic Reaction Mechanisms

Spatially and Temporally Resolved Measurements of NO Adsorption/Desorption over NOx‐Storage Catalyst

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