Hindered methane decomposition on a coke-resistant Ni-In/SiO2 dry reforming catalyst

Németh, Miklós; Sáfrán, György; Horváth, Anita; Somodi, Ferenc

doi:10.1016/j.catcom.2018.10.003

Cited by 29 publications

(20 citation statements)

References 20 publications

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“…Based on the above results and our previous publications on NiIn/SiO 2 , , the following statements can be drawn in connection with the dry reforming performance of the catalyst.…”

Section: Results and Discussionmentioning

confidence: 59%

Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

2019

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Recently a new In-promoted Ni catalyst has been elaborated and published in our laboratory, that has beneficial properties in dry reforming of methane, including inhibited coking. In order to get deeper insights into the coke-free behavior of this SiO 2 -supported 3 wt % Ni 2 wt % In catalyst, we wished to monitor the interaction between CO and the catalyst. For this purpose DRIFTS studies under CO, CO 2 , or CO 2 + CH 4 flow at different temperatures and CO pulse flow experiments at 600 °C followed by mass spectrometry were carried out. A linear carbonyl band at 2013 cm −1 in the DRIFT spectra of the In-promoted catalyst was attributed to CO bonded on Ni atoms surrounded by In neighbors. The lack of bridge and multicoordinated carbonyls also proved the dilution of Ni surface with In. In the presence of a CH 4 :CO 2 = 70:30 dry reforming mixture, stable Ni bonded CO species were found on NiIn/SiO 2 suggesting that the metallic sites remained clean during the reaction (unlike on the reference Ni/SiO 2 ). At the end of the reforming reaction, little surface segregation of the original bimetallic particles and the formation of islands with adjacent Ni sites were presumed based on the DRIFTS results. The pulse CO experiments at 600 °C, tailored to detect the most sensitive surface sites for Boudouard reaction, proved that CO dissociation on the bimetallic catalyst was markedly hindered, while it caused carbon deposition on the unpromoted sample. Based on all these results, we postulate a picture of the working catalyst that is dispersed ensembles of NiIn-InO x entities stabilized by SiO 2 .

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“…Based on the above results and our previous publications on NiIn/SiO 2 , , the following statements can be drawn in connection with the dry reforming performance of the catalyst.…”

Section: Results and Discussionmentioning

confidence: 59%

Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

2019

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“…However, the primary issue of the current catalysts is the deactivation owing to carbonaceous species or inactive carbon deposited on the catalysts during the reaction. This results from the formation of CH x ( x : 0–4) species attached to the catalyst surface owing to the decomposition of methane and CO disproportion . On the other side, the carbonaceous species may have developed through CH x dissociation in which the carbon atoms were diffused into the metal particle or polymerized on the surface of the catalyst .…”

Section: Introductionmentioning

confidence: 99%

High‐Performance Bimetallic Catalysts for Low‐Temperature Carbon Dioxide Reforming of Methane

et al. 2020

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Catalytic dry reforming of methane (DRM) is a promising way for renewable syngas production due to the utilization of both CO2 and CH4 greenhouse gases. Current approaches were made to improve the catalytic activity and coke resistance by introducing a second metal into the Ni‐based catalytic system. This bimetallic catalytic system showed a significant improvement in coke resistance due to the synergistic effect of both metals towards the reaction. This review summarizes recent developments in bimetallic catalysts in DRM which focused on the evaluation of catalysts, deactivation studies, and reaction mechanisms of developed bimetallic catalysts.

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“…[7] However, most of the existing catalysts using common oxide supports as well conventional nickel deposition routes face two important drawbacks: firstly metal sintering, which is accentuated by the high temperature at which the reaction has to be carried out due to thermodynamic reasons; [8,9] secondly, important formation of carbon deposits during the course of the reaction, due to the occurrence of CH 4 decomposition as side reaction [10,11] that leads to progressive activity loss by inhibiting the active sites and to plugging of the reactor when carbon nanotubes are formed in big amount. [12,13] In the last decade, numerous attempts like the use of a bimetallic catalyst [14][15][16] or altering the type of support [17,18] have been made to overcome these barriers and design more robust catalysts.…”

Section: Introductionmentioning

confidence: 99%

Porous Nickel‐Alumina Derived from Metal‐Organic Framework (MIL‐53): A New Approach to Achieve Active and Stable Catalysts in Methane Dry Reforming

et al. 2019

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An Al‐containing MIL‐53 metal‐organic framework with very high surface area (SBET=1130 m2.g−1, N2 sorption) was used as sacrificial template to prepare a nickel‐alumina‐based catalyst (Ni0AlMIL) highly active and stable in the reaction of dry reforming of methane (DRM). The procedure consisted in impregnating the activated (solvent free) MIL‐53 sample with a nickel precursor solution, then calcining the material to remove the organic linkers and subsequently reducing it to form the reduced nickel active phase. At the step of calcination, this procedure results in the formation of a porous uniform spinel phase with Ni nanospecies embedded in the alumina‐based matrix, as deduced from XRD, TPR and TEM analyses. This leads after reduction to a porous lamellar γ‐Al2O3 material with small Ni0 nanoparticles homogeneously dispersed and stabilized within the support. The performances of this catalyst in DRM are better than those of two reference Ni/alumina catalysts prepared for comparison by conventional nickel impregnation of two preformed alumina supports: a first one obtained by calcination of MIL‐53 (AlMIL) and a second one consisting of a commercial γ‐Al2O3 batch (AlCOM). Under steady state conditions at a temperature of 650 °C and a pressure of 1 bar, the higher CH4 and CO2 conversions (till 3 times higher than on Ni0/AlCOM), high catalytic stability (no loss of activity after 13–100 h) and higher selectivity towards DRM (H2:CO products ratio remaining at 1) on Ni0AlMIL compared to the other catalysts is believed to come from the particularly strong interaction between the nickel and alumina phases generated by using the unique high specific surface of the parent MOF support to deposit nickel. This creates an intimate mixing favorable to a persisting interaction of the nickel nanoparticles with the alumina support in the reduced material. The lamellar shape of the γ‐Al2O3 composing the catalyst and its remaining high specific surface may also contribute to the excellent Ni resistance to sintering and in turn to the inhibition of carbon nanotubes formation during the reaction.

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Hindered methane decomposition on a coke-resistant Ni-In/SiO2 dry reforming catalyst

Cited by 29 publications

References 20 publications

Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

High‐Performance Bimetallic Catalysts for Low‐Temperature Carbon Dioxide Reforming of Methane

Porous Nickel‐Alumina Derived from Metal‐Organic Framework (MIL‐53): A New Approach to Achieve Active and Stable Catalysts in Methane Dry Reforming

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Hindered methane decomposition on a coke-resistant Ni-In/SiO2 dry reforming catalyst

Cited by 29 publications

References 20 publications

Interaction between CO and a Coke-Resistant NiIn/SiO2 Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

Interaction between CO and a Coke-Resistant NiIn/SiO2 Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

High‐Performance Bimetallic Catalysts for Low‐Temperature Carbon Dioxide Reforming of Methane

Porous Nickel‐Alumina Derived from Metal‐Organic Framework (MIL‐53): A New Approach to Achieve Active and Stable Catalysts in Methane Dry Reforming

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Product

Resources

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Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study

Interaction between CO and a Coke-Resistant NiIn/SiO₂ Methane Dry Reforming Catalyst: A DRIFTS and CO Pulse Study