Dry Reforming of Methane at High Pressure in a Fixed-Bed Reactor with Axial Temperature Profile Determination

Tillmann, Lukas; Schulwitz, Jonas; Veen, A.C. van

doi:10.1007/s10562-018-2453-x

Cited by 25 publications

(10 citation statements)

References 11 publications

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“…For the activity measurements, the setup described in the work of Muhler et al was employed . The effluent gas was analyzed using an Agilent 3000 Micro-GC equipped with PLOT-Q and Molsieve 5A PLOT columns and a TCD for quantification.…”

Section: Methodsmentioning

confidence: 99%

In Situ X-ray Microscopy Reveals Particle Dynamics in a NiCo Dry Methane Reforming Catalyst under Operating Conditions

et al. 2020

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Herein, we report the synthesis of a γ-Al 2 O 3 -supported NiCo catalyst for dry methane reforming (DMR) and study the catalyst using in situ scanning transmission X-ray microscopy (STXM) during the reduction (activation step) and under reaction conditions. During the reduction process, the NiCo alloy particles undergo elemental segregation with Co migrating toward the center of the catalyst particles and Ni migrating to the outer surfaces. Under DMR conditions, the segregated structure is maintained, thus hinting at the importance of this structure to optimal catalytic functions. Finally, the formation of Ni-rich branches on the surface of the particles is observed during DMR, suggesting that the loss of Ni from the outer shell may play a role in the reduced stability and hence catalyst deactivation. These findings provide insights into the morphological and electronic structural changes that occur in a NiCo-based catalyst during DMR. Further, this study emphasizes the need to study catalysts under operating conditions in order to elucidate material dynamics during the reaction.

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Section: Methodsmentioning

confidence: 99%

In Situ X-ray Microscopy Reveals Particle Dynamics in a NiCo Dry Methane Reforming Catalyst under Operating Conditions

et al. 2020

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“…The DMR activity for the NiCoO/γ-Al 2 O 3 sample was reported in an earlier publication. 24 The experimental setup for measuring the activity of the NiO/γ-Al 2 O 3 DMR catalysts has been described in detail elsewhere by Tillmann et al, 24,36 Fig. S1.…”

Section: Dmr Activity Testsmentioning

confidence: 99%

In situ X-ray emission and high-resolution X-ray absorption spectroscopy applied to Ni-based bimetallic dry methane reforming catalysts

et al. 2020

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“…Because CRM is a highly endothermic reaction, it is usually operated at temperature range of 650 • C to 1000 • C [6,7]. A high temperature causes the short life of Ni-based catalysts mainly due to the metal sintering and the carbon formation, a by-product from side reactions including the Boudouard reaction (R2) and CH 4 decomposition (R3) [8,9]. Additionally, reverse water gas shift (RWGS) reaction (R4) is an another endothermic side reaction that decrease the hydrogen yield [10][11][12].…”

Section: Introductionmentioning

confidence: 99%

The Effect of ZrO2 as Different Components of Ni-Based Catalysts for CO2 Reforming of Methane and Combined Steam and CO2 Reforming of Methane on Catalytic Performance with Coke Formation

2021

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The role of ZrO2 as different components in Ni-based catalysts for CO2 reforming of methane (CRM) has been investigated. The 10 wt.% Ni supported catalysts were prepared with ZrO2 as a support using a co-impregnation method. As a promoter (1 wt.% ZrO2) and a coactive component (10 wt.% ZrO2), the catalysts with ZrO2 were synthesized using a co-impregnation method. To evaluate the effect of the interaction, the Ni catalyst with ZrO2 as a coactive component was prepared by a sequential impregnation method. The results revealed that the activity, the selectivity, and the anti-coking ability of the catalyst depend upon the ZrO2 content, the Ni-ZrO2 interaction, basicity, and oxygen mobility of each catalyst resulting in different Ni dispersion and oxygen transfer pathway from ZrO2 to Ni. According to the characterization and catalytic activation results, the Ni catalyst with low ZrO2 content (as a promoter) presented highest selectivity toward CO owning to the high number of weak and moderate basic sites that enhance the CO2 activation-dissociation. The lowest activity (CH4 conversion ≈ 40% and CO2 conversion ≈ 39%) with the relatively high quantity of total coke formation (the weight loss of the spent catalyst in TGA curve ≈ 22%) of the Ni catalyst with ZrO2 as a support is ascribed to the lowest Ni dispersion due to the poor Ni-ZrO2 interaction and less oxygen transfer from ZrO2 to the deposited carbon on the Ni surface. The effect of a poor Ni-ZrO2 interaction on the catalytic activity was deducted by decreasing ZrO2 content to 10 wt.% (as a coactive component) and 1 wt.% (as a promoter). Although Ni catalysts with 1 wt.% and 10 wt.% ZrO2 provided similar oxygen mobility, the lack of oxygen transfer to coke during CRM process on the Ni surface was still indicated by the growth of carbon filament when the catalyst was prepared by co-impregnation method. When the catalyst was prepared by a sequential impregnation, the intimate interaction of Ni and ZrO2 for oxygen transfer was successfully developed through a ZrO2-Al2O3 composite. The interaction in this catalyst enhanced the catalytic activity (CH4 conversion ≈ 54% and CO2 conversion ≈ 50%) and the oxygen transport for carbon oxidation (the weight loss of the spent catalyst in TGA curve ≈ 7%) for CRM process. The Ni supported catalysts with ZrO2 as a promoter prepared by co-impregnation and with ZrO2 as a coactive component prepared by a sequential impregnation were tested in combined steam and CO2 reforming of methane (CSCRM). The results revealed that the ZrO2 promoter provided a greater carbon resistance (coke = 1.213 mmol·g−1) with the subtraction of CH4 and CO2 activities (CH4 conversion ≈ 28% and CO2 conversion ≈ %) due to the loss of active sites to the H2O activation-dissociation. Thus, the H2O activation-dissociation was promoted more efficiently on the basic sites than on the vacancy sites in CSCRM.

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Dry Reforming of Methane at High Pressure in a Fixed-Bed Reactor with Axial Temperature Profile Determination

Abstract: Please refer to published version for the most recent bibliographic citation information. If a published version is known of, the repository item page linked to above, will contain details on accessing it.

Cited by 25 publications

References 11 publications

In Situ X-ray Microscopy Reveals Particle Dynamics in a NiCo Dry Methane Reforming Catalyst under Operating Conditions

In Situ X-ray Microscopy Reveals Particle Dynamics in a NiCo Dry Methane Reforming Catalyst under Operating Conditions

In situ X-ray emission and high-resolution X-ray absorption spectroscopy applied to Ni-based bimetallic dry methane reforming catalysts

The Effect of ZrO2 as Different Components of Ni-Based Catalysts for CO2 Reforming of Methane and Combined Steam and CO2 Reforming of Methane on Catalytic Performance with Coke Formation

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