Mechanism and kinetic modeling for steam reforming of toluene on La0.8Sr0.2Ni0.8Fe0.2O3 catalyst

Oemar, Usman; Li, Ang Ming; Hidajat, K.; Kawi, Sibudjing

doi:10.1002/aic.14573

Cited by 89 publications

(38 citation statements)

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“…The schematic of the setup was reported in our previous studies [26,34,35]. Briefly, the inlet section consisted of a specific concentration of To eliminate the mass-transfer effect, we selected a sample size of 100-150 mesh by providing the catalyst bed height to a catalyst particle size ratio of L/D p ≥ 50 and reactor internal diameter to a catalyst particle size ratio of D/D p ≥ 30 [36]. Catalytic ozonation of gaseous toluene over the MnO 2 /graphene sample was performed at varied temperatures (295, 313, and 333 K) under atmospheric pressure.…”

Section: Steady-state Kinetic Studymentioning

confidence: 99%

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Yao

Hui

et al. 2017

Chemical Engineering Journal

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This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. AbstractThe catalytic ozonation of VOCs is a promising approach for degradation of indoor VOCs, such as gaseous toluene. However, the mechanism and relevant kinetic steps involved in this reaction remain unclear. In this study, the catalytic ozonation of toluene over MnO 2 /graphene was investigated using the empirical power law model and classic Langmuir-Hinshelwood single-site (denoted as L-H s ) mechanism. The apparent activation energy determined using the power law model was 29.3±2.5 kJ mol −1 . This finding indicated that the catalytic ozonation of toluene over MnO 2 /graphene was a heterogeneous reaction, and the Langmuir-Hinshelwood mechanism was applicable. However, the L-H s mechanism did not fit the experimental data, suggesting that the reaction was non-single-site governed. A novel Langmuir-Hinshelwood dual-site (denoted as L-H d ) mechanism was then proposed to explain the experimental observations of the catalytic ozonation of toluene over MnO 2 /graphene through a steady-state kinetic study. This mechanism was based on the hypothesis that MnO 2 was responsible for ozone decomposition and toluene adsorption on graphene; these two types of adsorption were coupled by an adjacent attack. Furthermore, XPS results confirmed the presence of a strong connection between MnO 2 and graphene sites on the surface of MnO 2 /graphene. This connection allowed the adjacent attack and validated the dual-site mechanism. The L-H d model was consistent with the predicted reaction rate of toluene removal with a correlation coefficient near unity (r 2 = 0.9165). Moreover, the physical criterion was in accordance with both enthalpy and entropy of toluene adsorption constraints. Fulfillment of mathematical and physical criteria indicated the catalytic ozonation of toluene over MnO 2 /graphene can be well described by the L-H d mechanism. This study helps understand the catalytic ozonation of toluene over MnO 2 /graphene in a closely mechanistic view.

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Section: Steady-state Kinetic Studymentioning

confidence: 99%

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Yao

Hui

et al. 2017

Chemical Engineering Journal

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“…However, for NSL catalysts, some of the Sr is located between the Ni and the La 2 O 3 support, resulting in stronger interaction between the Ni and La 2 O 3 support. Our previous study 11,12 reported that Sr can adsorb and desorb more water at higher temperature than La, but only La can activate the water. Therefore, this study shows that the crucial role of Sr to strongly adsorb and desorb water can be enhanced by arranging Sr on the catalyst surface.…”

Section: Xps Of Reduced Catalystsmentioning

confidence: 99%

Enhancing performance of Ni/La₂O₃ catalyst by Sr-modification for steam reforming of toluene as model compound of biomass tar

et al. 2015

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Steam reforming of biomass tar with toluene as the model compound was studied using Sr-doped Ni/La 2 O 3 catalysts prepared using two methods, i.e. co-impregnation of Sr and Ni on La 2 O 3 support (Ni-Sr/La 2 O 3 catalyst) and sequential impregnation of Sr on Ni/La 2 O 3 catalyst (SNL catalyst), which were then calcined at various temperatures (500, 700, and 900 C). These two types of catalysts are found to possess better catalytic performance than the undoped Ni/La 2 O 3 catalyst at the same calcination temperature due to the presence of Sr, which helps in water adsorption at low steam/carbon (S/C) ratio. Moreover, the catalytic performance for catalysts calcined at various temperatures decreases following this trend: 500 C > 700 C > 900 C due to lower BET surface area and lower surface active metal available for reaction. In addition, it is also observed that the Sr/Ni/La 2 O 3 catalyst has better performance than the Ni-Sr/La 2 O 3 catalyst at the same calcination temperature. Further characterization results suggest that in the Ni-Sr/La 2 O 3 catalyst, the Sr is present between Ni and La 2 O 3 support. On the other hand, Sr in the Sr/Ni/La 2 O 3 catalyst is thought to be located on the surface of Ni/La 2 O 3 due to the preparation method. This study shows that more Sr on the catalyst surface has better catalytic activity and stability in steam reforming of toluene. IntroductionThe need for a renewable alternative of energy sources is increasingly urgent due to the rapid depletion of fossil fuel reserves and the costly price tag of crude oil. The utilization of biomass has been receiving more attention as an abundant and cheap source of renewable energy. Among them, biomass gasication has garnered considerable attention for hydrogen/ synthesis gas production, which can then be used for Fischer Tropsch processes, syntheses of methanol and electricity production in the case of a fuel cell. [1][2][3][4] The main challenge in biomass gasication technology is the removal of tar, which is a mixture of various condensable hydrocarbon compounds containing toluene as the major component, followed by naphthalene. 3 Furthermore, tar can polymerize to form more complex structures and aerosols. Tar can condense on particulate lters, heat exchangers, and engines, resulting in plugging and attrition. This further causes a decrease in efficiency of the process operations and an increase in maintenance and operating costs. Tar removal methods can be classied as primary or secondary. Primary methods include all measures taken in the gasication reactor to prevent tar from being formed in the gasier or to convert it.In secondary methods, pretreatment, either chemical or physical, is performed downstream of the gasier. Both primary and secondary methods require the use of a catalyst.Various metal catalysts have been investigated, such as Ni 5-12 Co, [13][14][15][16][9][10][11][12][16][17][18] and noble metal 19 for the steam reforming of biomass tar using toluene as the model compound. Among those metal catalysts, Ni cataly...

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“…Oxygen affinity of Ce improved the activity of Ni/Al 2 O 3 catalyst in terms of coke suppression. Adsorbed O species in presence of Ce and Ni, due to lattice O and redox properties of Ce forms gas species such as CO 2 and CO instead of coke deposition (Oemar et al, 2014). Fig.…”

Section: Effect Of Catalysts On Product Distributionmentioning

confidence: 99%

Ceria promoted deoxygenation and denitrogenation of Thalassiosira weissflogii and its model compounds by catalytic in-situ pyrolysis

Aysu

Maroto‐Valer

Sanna

2016

Bioresource Technology

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Mechanism and kinetic modeling for steam reforming of toluene on La_0.8Sr_0.2Ni_0.8Fe_0.2O₃ catalyst

Cited by 89 publications

References 60 publications

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Enhancing performance of Ni/La₂O₃ catalyst by Sr-modification for steam reforming of toluene as model compound of biomass tar

Ceria promoted deoxygenation and denitrogenation of Thalassiosira weissflogii and its model compounds by catalytic in-situ pyrolysis

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Mechanism and kinetic modeling for steam reforming of toluene on La0.8Sr0.2Ni0.8Fe0.2O3 catalyst

Cited by 89 publications

References 60 publications

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Novel mechanistic view of catalytic ozonation of gaseous toluene by dual-site kinetic modelling

Enhancing performance of Ni/La2O3 catalyst by Sr-modification for steam reforming of toluene as model compound of biomass tar

Ceria promoted deoxygenation and denitrogenation of Thalassiosira weissflogii and its model compounds by catalytic in-situ pyrolysis

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Mechanism and kinetic modeling for steam reforming of toluene on La_0.8Sr_0.2Ni_0.8Fe_0.2O₃ catalyst

Enhancing performance of Ni/La₂O₃ catalyst by Sr-modification for steam reforming of toluene as model compound of biomass tar