Global Reaction Kinetics of CO and CO<sub>2</sub> Methanation for Dynamic Process Modeling

Rönsch, Stefan; Köchermann, Jakob; Schneider, Jens; Matthischke, Steffi

doi:10.1002/ceat.201500327

Cited by 75 publications

(47 citation statements)

References 33 publications

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“…Those profiles are in accordance with data published by Harms et al . Detailed information regarding the validation of the stationary state profiles can be found in .…”

Section: Resultssupporting

confidence: 89%

“…The rate of CO methanation (Eq. ) is calculated according to Rönsch et al , who proposed an adaption of the rate determined by Klose for commercial 18 % nickel methanation catalysts.

true r_{normalMETH} = - \frac{k_{1} K_{normalC} K_{normalH}^{2} p_{normalCO}^{0.5} p_{{normalH}_{2}}}{{(1 + K_{normalC} p_{normalCO}^{0.5} + K_{normalH} p_{{normalH}_{2}}^{0.5})}^{3}} + \frac{k_{1} K_{normalC} K_{normalH}^{2} p_{normalC {normalH}_{4}} p_{{normalH}_{2} normalO} p_{normalCO}^{- 0.5} p_{{normalH}_{2}}^{- 2} (\frac{1}{K_{METH}})}{{(1 + K_{normalC} p_{normalCO}^{0.5} + K_{normalH} p_{{normalH}_{2}}^{0.5})}^{3}}

…”

Section: Modeling and Simulationmentioning

confidence: 99%

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Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

2017

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The production of synthetic natural gas (SNG) from renewable sources in cases requires a dynamic and intermitted operation of the methanation reactors. This may lead to catalyst damage. Therefore, the present work is aiming at identifying restrictions and optimization approaches of the start‐and‐stop operation of fixed‐bed methanation reactors. 2D modeling and simulation work is conducted and the warm‐start behavior of a fixed‐bed reactor after one to four hours operation intermittence is analyzed. The result reveals the possibility for an operation interruption of up to four hours without high adaptation effort to restart the reactor. After approximately four hours, the catalyst bed at the inlet part of the reactor reaches a temperature that provokes problems for a subsequent warm start.

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“…Those profiles are in accordance with data published by Harms et al . Detailed information regarding the validation of the stationary state profiles can be found in .…”

Section: Resultssupporting

confidence: 89%

“…The rate of CO methanation (Eq. ) is calculated according to Rönsch et al , who proposed an adaption of the rate determined by Klose for commercial 18 % nickel methanation catalysts.

true r_{normalMETH} = - \frac{k_{1} K_{normalC} K_{normalH}^{2} p_{normalCO}^{0.5} p_{{normalH}_{2}}}{{(1 + K_{normalC} p_{normalCO}^{0.5} + K_{normalH} p_{{normalH}_{2}}^{0.5})}^{3}} + \frac{k_{1} K_{normalC} K_{normalH}^{2} p_{normalC {normalH}_{4}} p_{{normalH}_{2} normalO} p_{normalCO}^{- 0.5} p_{{normalH}_{2}}^{- 2} (\frac{1}{K_{METH}})}{{(1 + K_{normalC} p_{normalCO}^{0.5} + K_{normalH} p_{{normalH}_{2}}^{0.5})}^{3}}

…”

Section: Modeling and Simulationmentioning

confidence: 99%

Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

2017

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“…Simulations of dynamic methanation reactors have been conducted to gain kinetic data and to address problems such as overheating during the transient process [25,26]. Other systems that have been studied under transient reaction conditions are, e.g., the Fischer-Tropsch reaction, where the influence of unsteady state conditions on the process itself was investigated [7,8,27].…”

Section: Introductionmentioning

confidence: 99%

Surface Oxidation of Supported Ni Particles and Its Impact on the Catalytic Performance during Dynamically Operated Methanation of CO2

et al. 2017

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Abstract:The methanation of CO 2 within the power-to-gas concept was investigated under fluctuating reaction conditions to gather detailed insight into the structural dynamics of the catalyst. A 10 wt % Ni/Al 2 O 3 catalyst with uniform 3.7 nm metal particles and a dispersion of 21% suitable to investigate structural changes also in a surface-sensitive way was prepared and characterized in detail. Operando quick-scanning X-ray absorption spectroscopy (XAS/QEXAFS) studies were performed to analyze the influence of 30 s and 300 s H 2 interruptions during the methanation of CO 2 in the presence of O 2 impurities (technical CO 2 ). These conditions represent the fluctuating supply of H 2 from renewable energies for the decentralized methanation. Short-term H 2 interruptions led to oxidation of the most reactive low-coordinated metallic Ni sites, which could not be re-reduced fully during the subsequent methanation cycle and accordingly caused deactivation. Detailed evaluation of the extended X-ray absorption fine structure (EXAFS) spectra showed surface oxidation/reduction processes, whereas the core of the Ni particles remained reduced. The 300-s H 2 interruptions resulted in bulk oxidation already after the first cycle and a more pronounced deactivation. These results clearly show the importance and opportunities of investigating the structural dynamics of catalysts to identify their mechanism, especially in power-to-chemicals processes using renewable H 2 .

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“…Such studies of the recirculation ratio are especially meaningful when CB models with spatial discretization and realistic methanation kinetics are applied (Rönsch, Köchermann, et al 2016) so that local hot spots can be located and their formation effectively controlled.…”

Section: Discussionmentioning

confidence: 99%

Dynamic simulation of a decentralized polygeneration plant providing SNG, steam and power

Schneider

Rothfuss

Rönsch

2016

International Journal of Sustainable Engineering

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The behaviour of a decentralized polygeneration plant providing synthetic natural gas (SNG), steam and electrical power is simulated in three scenarios in this study. The plant size is based on an assumed capacity of decentralized polygeneration plants processing 1070 m 3 h −1 (STP) of syngas. 396 m 3 h −1 (STP) of raw SNG, 0.4 t h −1 of steam at 5 bar and 670 kW of electrical power can be generated by the plant at the reference scenario. Methanation reactor and steam generator are modelled in detail. Further results indicate that such a polygeneration plant can provide positive and negative operation reserves for the electricity network to the extent of 100% of the reference power output, while the amount of generated steam varies by less than 40%. At the same time, the generated SNG quality keeps constant. Lower variations in the amount of generated steam are applicable when reducing the operation reserve capacity.

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Global Reaction Kinetics of CO and CO₂ Methanation for Dynamic Process Modeling

Cited by 75 publications

References 33 publications

Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

Surface Oxidation of Supported Ni Particles and Its Impact on the Catalytic Performance during Dynamically Operated Methanation of CO2

Dynamic simulation of a decentralized polygeneration plant providing SNG, steam and power

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Global Reaction Kinetics of CO and CO2 Methanation for Dynamic Process Modeling

Cited by 75 publications

References 33 publications

Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

Start‐and‐Stop Operation of Fixed‐Bed Methanation Reactors – Results from Modeling and Simulation

Surface Oxidation of Supported Ni Particles and Its Impact on the Catalytic Performance during Dynamically Operated Methanation of CO2

Dynamic simulation of a decentralized polygeneration plant providing SNG, steam and power

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Product

Resources

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Global Reaction Kinetics of CO and CO₂ Methanation for Dynamic Process Modeling