Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier
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The implementation of the liquid organic hydrogen carrier (LOHC) technology for efficient energy storage requires the development of a reliable kinetic model for both hydrogenation and dehydrogenation processes. In this research study, the catalytic hydrocarbon saturation for a dibenzyltoluene (DBT) mixture solution, containing dibenzylbenzene (DBB), dibenzylethylbenzene (DBEB) and impurities has been performed in the presence of Ru/Al2O3 particles. The influence of different reaction conditions, such as temperature, pressure, initial reactant concentration, catalyst amount and stirring speed has been examined. A measurement-based system micro-kinetics, based on the Langmuir–Hinshelwood mechanism with dissociative H2 surface adsorption, has been derived. H2 thermodynamic solubility equilibrium was defined through Henry's law. The adsorbing, desorption and reactivity of inert solvent molecules was not considered to be relevant. The mass transfer resistance over 1000 rpm stirring speed w...as negligible. Relative- and mean squared error of representation were 40.9% and 1.00×10−4, respectively. Expressions gave an excellent data prediction for the profile period trends with a relatively accurate estimation of H2 intermediates' rate selectivity, H2-covered area approximation and pathway rate-determining steps. Due to the lack of commercially available standard chemical compounds for quantitative analysis techniques, a novel experiment-based numerical calibration method was developed. Mean field (micro)kinetics represent an advancement in the mesoscale mechanistic understanding of physical interface phenomena. This also enables catalysis structure–activity relationships, unlocking the methodology for new LOHC reaching beyond traditional, such as ammonia, methanol and formate, which do not release H2 alone. Integrated multiscale simulations could include fluidics later on.
Keywords:
Dibenzyltoluene / Hydrogenation / Langmuir-Hinshelwood kinetics / Liquid organic hydrogen carrier / Reaction kinetics modelingSource:
Applied Energy, 07-2024, 365, 123262-Publisher:
- Elsevier Ltd.
Funding / projects:
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia, institutional funding - 200135 (University of Belgrade, Faculty of Technology and Metallurgy) (RS-MESTD-inst-2020-200135)
- Ministry of Science, Technological Development and Innovation of the Republic of Serbia (Contract No. 451-03-1271/2022-14/ 3131)
- Programme P2-152, projects N2-0291, N2-0316, J7-4638 and HYBREED
Institution/Community
Tehnološko-metalurški fakultetTY - JOUR AU - Tomić, Aleksandra AU - Pomeroy, Brett AU - Todić, Branislav AU - Likozar, Blaž AU - Nikačević, Nikola PY - 2024-07 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/7452 AB - The implementation of the liquid organic hydrogen carrier (LOHC) technology for efficient energy storage requires the development of a reliable kinetic model for both hydrogenation and dehydrogenation processes. In this research study, the catalytic hydrocarbon saturation for a dibenzyltoluene (DBT) mixture solution, containing dibenzylbenzene (DBB), dibenzylethylbenzene (DBEB) and impurities has been performed in the presence of Ru/Al2O3 particles. The influence of different reaction conditions, such as temperature, pressure, initial reactant concentration, catalyst amount and stirring speed has been examined. A measurement-based system micro-kinetics, based on the Langmuir–Hinshelwood mechanism with dissociative H2 surface adsorption, has been derived. H2 thermodynamic solubility equilibrium was defined through Henry's law. The adsorbing, desorption and reactivity of inert solvent molecules was not considered to be relevant. The mass transfer resistance over 1000 rpm stirring speed was negligible. Relative- and mean squared error of representation were 40.9% and 1.00×10−4, respectively. Expressions gave an excellent data prediction for the profile period trends with a relatively accurate estimation of H2 intermediates' rate selectivity, H2-covered area approximation and pathway rate-determining steps. Due to the lack of commercially available standard chemical compounds for quantitative analysis techniques, a novel experiment-based numerical calibration method was developed. Mean field (micro)kinetics represent an advancement in the mesoscale mechanistic understanding of physical interface phenomena. This also enables catalysis structure–activity relationships, unlocking the methodology for new LOHC reaching beyond traditional, such as ammonia, methanol and formate, which do not release H2 alone. Integrated multiscale simulations could include fluidics later on. PB - Elsevier Ltd. T2 - Applied Energy T1 - Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier SP - 123262 VL - 365 DO - 10.1016/j.apenergy.2024.123262 ER -
@article{ author = "Tomić, Aleksandra and Pomeroy, Brett and Todić, Branislav and Likozar, Blaž and Nikačević, Nikola", year = "2024-07", abstract = "The implementation of the liquid organic hydrogen carrier (LOHC) technology for efficient energy storage requires the development of a reliable kinetic model for both hydrogenation and dehydrogenation processes. In this research study, the catalytic hydrocarbon saturation for a dibenzyltoluene (DBT) mixture solution, containing dibenzylbenzene (DBB), dibenzylethylbenzene (DBEB) and impurities has been performed in the presence of Ru/Al2O3 particles. The influence of different reaction conditions, such as temperature, pressure, initial reactant concentration, catalyst amount and stirring speed has been examined. A measurement-based system micro-kinetics, based on the Langmuir–Hinshelwood mechanism with dissociative H2 surface adsorption, has been derived. H2 thermodynamic solubility equilibrium was defined through Henry's law. The adsorbing, desorption and reactivity of inert solvent molecules was not considered to be relevant. The mass transfer resistance over 1000 rpm stirring speed was negligible. Relative- and mean squared error of representation were 40.9% and 1.00×10−4, respectively. Expressions gave an excellent data prediction for the profile period trends with a relatively accurate estimation of H2 intermediates' rate selectivity, H2-covered area approximation and pathway rate-determining steps. Due to the lack of commercially available standard chemical compounds for quantitative analysis techniques, a novel experiment-based numerical calibration method was developed. Mean field (micro)kinetics represent an advancement in the mesoscale mechanistic understanding of physical interface phenomena. This also enables catalysis structure–activity relationships, unlocking the methodology for new LOHC reaching beyond traditional, such as ammonia, methanol and formate, which do not release H2 alone. Integrated multiscale simulations could include fluidics later on.", publisher = "Elsevier Ltd.", journal = "Applied Energy", title = "Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier", pages = "123262", volume = "365", doi = "10.1016/j.apenergy.2024.123262" }
Tomić, A., Pomeroy, B., Todić, B., Likozar, B.,& Nikačević, N.. (2024-07). Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier. in Applied Energy Elsevier Ltd.., 365, 123262. https://doi.org/10.1016/j.apenergy.2024.123262
Tomić A, Pomeroy B, Todić B, Likozar B, Nikačević N. Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier. in Applied Energy. 2024;365:123262. doi:10.1016/j.apenergy.2024.123262 .
Tomić, Aleksandra, Pomeroy, Brett, Todić, Branislav, Likozar, Blaž, Nikačević, Nikola, "Catalytic hydrogenation reaction micro-kinetic model for dibenzyltoluene as liquid organic hydrogen carrier" in Applied Energy, 365 (2024-07):123262, https://doi.org/10.1016/j.apenergy.2024.123262 . .