Heterogeneous chemical reactions—A cornerstone in emission reduction of local pollutants and greenhouse gases

Lott, Patrick; Deutschmann, Olaf

doi:10.1016/j.proci.2022.06.001

Cited by 29 publications

(10 citation statements)

References 272 publications

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“…In order to overcome these boundaries, both the experimental foundation and the simulation of these phenomena need to be improved. Although global kinetics are mostly limited to the described setup environment they are developed for, their formulation allows to capture and compare the frequently studied water effects on methane oxidation over different support materials typically with higher cost and time efficiency than microkinetic models [21] …”

Section: Introductionmentioning

confidence: 99%

“…Although global kinetics are mostly limited to the described setup environment they are developed for, their formulation allows to capture and compare the frequently studied water effects on methane oxidation over different support materials typically with higher cost and time efficiency than microkinetic models. [21] This work aims at deepening the understanding of the total methane oxidation and underlying water inhibition effect on PdO-based catalysts. For this, powder-bed experiments with Pdcatalysts supported on Al 2 O 3 , CeO 2 , SnO 2 , and ZrO 2 were conducted in the absence and presence of steam, which provides a solid database for discussing the water inhibition effect.…”

Section: Introductionmentioning

confidence: 99%

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Methane Oxidation over PdO: Towards a Better Understanding of the Influence of the Support Material

et al. 2023

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The presence of water vapor during the oxidation of the strong greenhouse gas methane over PdO‐based catalysts is known to result in severe inhibition and catalyst deactivation. In this context, our current study elucidates the role of the support material for different water concentrations in the reaction gas mixture. Compared to a reference PdO/Al2O3 catalyst, the catalytic activity can be significantly enhanced when using SnO2 and ZrO2 as support materials and remains stable during 24 h of operation at 823 K in the presence of 12 % H2O, whereas under identical conditions CH4 conversion drops by 68 % over PdO/Al2O3. The interplay between Pd species and catalyst support was systematically characterized by thermogravimetric analysis, temperature‐programmed reduction experiments and TEM measurements. Finally, a kinetic scheme was derived based on the experimental data.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Methane Oxidation over PdO: Towards a Better Understanding of the Influence of the Support Material

et al. 2023

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“…Characteristic aspects of homogeneous/heterogeneous reaction systems can be analyzed with combinations of gas-phase diagnostics (Section ) and techniques from surface science. Several recent reviews and perspectives provide excellent introductions into methods, status, and research needs of the field. − Detailed investigations of catalytic reactions in a combustion context can profit from the analytical expertise obtained from inspection of gas-phase combustion systems, , e.g., by employing VUV-PI-MBMS to analyze the selective conversion of syngas to light olefins, or PEPICO spectroscopy for tracing gas-phase radicals (Section ) in a study of light alkane functionalization, in which this technique was coupled with operando spectroscopy and DFT calculations …”

Section: Developments For Systems and Applicationsmentioning

confidence: 99%

Combustion, Chemistry, and Carbon Neutrality

Kohse‐Höinghaus

2023

Chem. Rev.

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Combustion is a reactive oxidation process that releases energy bound in chemical compounds used as fuels�energy that is needed for power generation, transportation, heating, and industrial purposes. Because of greenhouse gas and local pollutant emissions associated with fossil fuels, combustion science and applications are challenged to abandon conventional pathways and to adapt toward the demand of future carbon neutrality. For the design of efficient, low-emission processes, understanding the details of the relevant chemical transformations is essential. Comprehensive knowledge gained from decades of fossil-fuel combustion research includes general principles for establishing and validating reaction mechanisms and process models, relying on both theory and experiments with a suite of analytic monitoring and sensing techniques. Such knowledge can be advantageously applied and extended to configure, analyze, and control new systems using different, nonfossil, potentially zero-carbon fuels. Understanding the impact of combustion and its links with chemistry needs some background. The introduction therefore combines information on exemplary cultural and technological achievements using combustion and on nature and effects of combustion emissions. Subsequently, the methodology of combustion chemistry research is described. A major part is devoted to fuels, followed by a discussion of selected combustion applications, illustrating the chemical information needed for the future.

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“…This requires the estimation of rate constants of all such elementary steps and a numerical solution of the governing equations for surface and fluid species, making parameter estimation a necessary step for successful microkinetic modeling. The kinetic and thermochemical values may typically be obtained from computational methods such as density functional theory (DFT) or through more empirical methods like bond-order conservation (BOC) method and Brønsted–Evans–Polanyi (BEP) relationships. − However, an accurate determination of the many kinetic parameters needed when choosing the MKM approach is a limiting factor . Additionally, MKM models do not directly account for the influence of supports or promoters on the kinetic parameters, therefore, the simulation data often does not agree well with experimental data for other catalyst/support material systems, requiring further fine-tuning of the mechanism.…”

Section: Introductionmentioning

confidence: 99%

Automating the Optimization of Catalytic Reaction Mechanism Parameters Using Basin-Hopping: A Proof of Concept

et al. 2023

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Parameter estimation is a crucial step for successful microkinetic modeling in catalysis. However, the large number of parameters to be optimized in order to match the experimental data is a bottleneck. In this regard, the global optimization algorithm Basin-Hopping is utilized to automate the typically time-extensive and error-prone task of manual fitting of kinetic parameters for a heterogeneous catalytic system. The stochastic approach of the Basin-Hopping algorithm to explore the kinetic parameter solution space coupled with local search methods makes it possible to screen the high-dimensional space for an optimal set of kinetic parameters giving the least residual between the simulated and the experimentally measured catalytic performance data. Our approach also ensures that only thermodynamically consistent solution candidates are explored at each optimization step. We utilize two example case studies in heterogeneous catalysis, namely, methane oxidation over a palladium catalyst and carbon monoxide methanation over a nickel catalyst, with corresponding detailed kinetic models to illustrate the applicability of the algorithm to efficiently fine-tune detailed kinetic models.

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Heterogeneous chemical reactions—A cornerstone in emission reduction of local pollutants and greenhouse gases

Cited by 29 publications

References 272 publications

Methane Oxidation over PdO: Towards a Better Understanding of the Influence of the Support Material

Methane Oxidation over PdO: Towards a Better Understanding of the Influence of the Support Material

Combustion, Chemistry, and Carbon Neutrality

Automating the Optimization of Catalytic Reaction Mechanism Parameters Using Basin-Hopping: A Proof of Concept

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