Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/γ-Al&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;3&lt;/sub&gt; Catalysts during the Direct Dehydrogenation of Isobutane

Sugiyama, Shigeru; Oribe, Kenta; Endo, Shino; Yoshida, Tashu; Shimoda, Naohiro; Katoh, Masahiro; Kato, Yuki; Ninomiya, Wataru

doi:10.1252/jcej.20we198

Cited by 4 publications

(9 citation statements)

References 19 publications

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“…Despite this normal background, when dehydrogenation of isobutane to isobutene was performed in our labora-tory using a NiO/γ-Al 2 O 3 catalyst, we found that the isobutene yield improved signi cantly with time-on-stream (Sugiyama et al, 2021). Because on the supported catalyst nickel oxide is reduced to metallic Ni at the initial stage of the reaction, the metallic nickel species becomes the active catalytic site.…”

Section: Introductionmentioning

confidence: 84%

“…1.1 Preparation of the catalysts e catalyst referred to as NiO(x)/γ-Al 2 O 3 , in which "x" indicates the content by weight %, de ned as 100×NiO [g]/ (γ-Al 2 O 3 [g]+NiO [g]), was prepared via the impregnation method, as previously reported (Ding et al, 2010a;Sugiyama et al, 2021). As an example of the catalyst preparation, the method used to prepare NiO(5)/γ-Al 2 O 3 is as follows.…”

Section: Methodsmentioning

confidence: 99%

“…However, using NiO(13)/γ-Al 2 O 3 and NiO(15)/γ-Al 2 O 3 , the yield of ethylene was increased to 2.0 and 3.25 h on-stream, respectively, and then decreased. Furthermore, when NiO(18)/γ-Al 2 O 3 and NiO(20)/γ-Al 2 O 3 were used, the yield of ethylene increased with time-onstream and showed the same behavior as the catalytic dehydrogenation of isobutane (Sugiyama et al, 2021). On the other hand, NiO(30)/γ-Al 2 O 3 showed no activity.…”

Section: Catalytic Performancesmentioning

confidence: 97%

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Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/Al2O3 during the Dehydrogenation of Ethane and Propane

Sugiyama

Koizumi

Iwaki

et al. 2022

J. Chem. Eng. Japan

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The dehydrogenation of isobutane to isobutene was accomplished using a NiO/γ-Al 2 O 3 catalyst. Furthermore, signi cant improvement in the time-on-stream yield of isobutene was achieved. During the normal catalytic dehydrogenation of alkanes, the catalyst is covered by carbon deposition generated during the reaction, which signi cantly reduces the activity with time-on-stream. Therefore, no examples of the catalytic dehydrogenation of isobutane have yet been reported. This study used either ethane or propane as a source of isobutane to examine whether the activity was improved with time-on-stream. As a result, in the dehydrogenations of both ethane and propane on a NiO/γ-Al 2 O 3 catalyst, the catalytic activity decreased with time-on-stream when the supporting amount of NiO was small. In contrast, when the supporting amount of NiO was large, the catalytic activity improved with time-on-stream. Using a NiO/γ-Al 2 O 3 catalyst with small and large NiO loadings led to similar results to those of isobutane dehydrogenation. In addition, it was con rmed that the dehydrogenation activity was improved with time-on-stream in the catalytic dehydrogenations of ethane, propane, and isobutane using high NiO loadings. The behavior using a moderate amount of NiO loading, which was not detected in the dehydrogenation of isobutane, was also observed, which resulted in a maximum yield of either ethylene or propylene at 2.0 or 3.25 h on-stream, respectively. We concluded that the reason the catalytic activity did not improve with time-on-stream when using a NiO/γ-Al 2 O 3 catalyst was because the supporting amount of NiO was negligible. These results demonstrate that the activity with time-on-stream could also be improved in the dehydrogenations of other alkanes.

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Section: Introductionmentioning

confidence: 84%

Section: Methodsmentioning

confidence: 99%

Section: Catalytic Performancesmentioning

confidence: 97%

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Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/Al2O3 during the Dehydrogenation of Ethane and Propane

Sugiyama

Koizumi

Iwaki

et al. 2022

J. Chem. Eng. Japan

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“…The coke formed at the catalyst surface is considered as one of the major factors negatively affecting the catalytic activity of all catalytic processes. However, Sugiyama et al [225] recently reported the positive effect of coke formation. They investigated Ni/γ-Al 2 O 3 and Cr 2 O 3 /γ-Al 2 O 3 catalysts for direct dehydrogenation of isobutane.…”

Section: Conclusion and Future Perspectivesmentioning

confidence: 99%

“…It is generally accepted that the catalytic activity of nickel catalysts is strictly connected with the size of the nickel particles: the smaller the Ni particles, the better the catalytic activity, resulting from the stronger active metal-support interactions, delayed sintering, and a lower rate of formation of carbon deposits [3,5,14,225]. However, in the case of molybdenum carbide supported nickel catalysts, the ratio of Ni/Mo to the size of nickel particles plays a predominant role [51,226].…”

Section: Molybdenum Carbide Modified With Nickel Particlesmentioning

confidence: 99%

Metal (Mo, W, Ti) Carbide Catalysts: Synthesis and Application as Alternative Catalysts for Dry Reforming of Hydrocarbons—A Review

Czaplicka

Rogala

Wysocka

2021

IJMS

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Dry reforming of hydrocarbons (DRH) is a pro-environmental method for syngas production. It owes its pro-environmental character to the use of carbon dioxide, which is one of the main greenhouse gases. Currently used nickel catalysts on oxide supports suffer from rapid deactivation due to sintering of active metal particles or the deposition of carbon deposits blocking the flow of gases through the reaction tube. In this view, new alternative catalysts are highly sought after. Transition metal carbides (TMCs) can potentially replace traditional nickel catalysts due to their stability and activity in DR processes. The catalytic activity of carbides results from the synthesis-dependent structural properties of carbides. In this respect, this review presents the most important methods of titanium, molybdenum, and tungsten carbide synthesis and the influence of their properties on activity in catalyzing the reaction of methane with carbon dioxide.

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Carbon Deposition Assisting the Enhancement of Catalytic Activity with Time-on-Stream in the Dehydrogenation of Isobutane over NiO/Al2O3

Sugiyama

Yoshida

Shimoda

et al. 2022

J. Chem. Eng. Japan

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In the transformation reaction of alkanes in alkenes via catalytic dehydrogenation, it is generally accepted that catalytic deactivation will occur. This phenomenon causes a drastic reduction in the catalytic activity with time-on-stream. It is understood that carbon deposits generated during the reaction then covers the surface of the catalyst, leading to a drastic decrease in activity. However, in contradiction, our laboratory reported that the dehydrogenation of isobutane to isobutene on NiO/γ-Al 2 O 3 within a speci c range of NiO loading with CO 2 improved the yield of isobutene with timeon-stream. Since few such cases have been reported, in this study, isobutane was dehydrogenated with CO 2 over the NiO/α-Al 2 O 3 catalyst, with 20% NiO loading, and an improvement was again observed. To investigate the cause of the improvement, both NiO/γ-Al 2 O 3 and NiO/α-Al 2 O 3 with 20% NiO loading were examined in detail following the reaction. According to transmission electron microscopy (TEM) analysis, both catalysts were covered with a large amount of carbon deposit after the reaction; however, there was a di erence in the types. The carbon deposit on NiO/γ-Al 2 O 3 exhibited a brous nature, while that on NiO/α-Al 2 O 3 appeared to be a type of nanowire. Raman spectroscopy revealed that the carbonaceous crystal-growth properties of the two forms di ered depending on the support. In particular, a catalytically active species of metallic nickel was formed in a high degree of dispersion in and on the above two forms of carbon deposits during the reaction, and this resulted in a high catalytic activity even when the catalyst was covered with a carbon deposit.

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Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/γ-Al<sub>2</sub>O<sub>3</sub> Catalysts during the Direct Dehydrogenation of Isobutane

Cited by 4 publications

References 19 publications

Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/Al<sub>2</sub>O<sub>3</sub> during the Dehydrogenation of Ethane and Propane

Enhancement of the Catalytic Activity Associated with Carbon Deposition Formed on NiO/Al<sub>2</sub>O<sub>3</sub> during the Dehydrogenation of Ethane and Propane

Metal (Mo, W, Ti) Carbide Catalysts: Synthesis and Application as Alternative Catalysts for Dry Reforming of Hydrocarbons—A Review

Carbon Deposition Assisting the Enhancement of Catalytic Activity with Time-on-Stream in the Dehydrogenation of Isobutane over NiO/Al<sub>2</sub>O<sub>3</sub>

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