Active phase, catalytic activity, and induction period of Fe/zeolite material in nonoxidative aromatization of methane

Tan, P. L.

doi:10.1016/j.jcat.2016.01.027

Cited by 244 publications

(141 citation statements)

References 39 publications

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“…PtBi catalyst had also higher selectivity to C 2 products, and PtSn catalyst exhibited similar selectivity to detected products. The most comparable is 2% Fe/HZSM‐5 catalyst prepared by Tan . Conversion of CH 4 was higher, which is expected since experiments were conducted lower WHSV and higher temperature.…”

Section: Resultsmentioning

confidence: 85%

“…Specific surface area (S BET ) of the parent HZSM‐5 was 348 m 2 /g. As it is usual when metal is loaded onto a zeolite, the specific surface area of all prepared catalysts decreased compared with the parent zeolite. The largest decrease in S BET , 49 m 2 /g, was observed for 2.5% Mo catalyst.…”

Section: Resultsmentioning

confidence: 86%

“…When metal is loaded into zeolite, the metal species can exchange with protons on Brønsted acid sites during the preparation of catalyst and therefore occupy the sites that become unavailable for NH 3 adsorption. Decrease of the high temperature peak for 2.5% Fe/HZSM‐5 is a consequence of Fe ions exchange with protons on Brønsted acid sites, which happens during preparation . The decrease of the high temperature peak in the case of Mo catalyst is not so evident.…”

Section: Resultsmentioning

confidence: 94%

“…Two carbenes stabilized this way can couple to ethylene. Further aromatization is possible on Brønsted acid sites . Before the catalyst is activated, methane is mainly consumed for reduction, and CO 2 , CO, H 2 O, and H 2 are the main products.…”

Section: Resultsmentioning

confidence: 99%

“…Monometallic and bimetallic Mo and Fe catalysts were prepared on HZSM-5 support with SiO 2 /Al 2 O 3 ratio 30. In contrast to already published works, [15][16][17][18][19][20][21][22][23] where similar catalysts were prepared and evaluated for MDA reaction, our aim was to achieve production of ethylene and ethane over a longer period of TOS. We also report the promotional effect of Fe addition to Mo on methane conversion and a relatively stable Fe catalyst for nonoxidative conversion of methane to C 2 products.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

Nonoxidative methane activation, coupling, and conversion to ethane, ethylene, and hydrogen over Fe/HZSM‐5, Mo/HZSM‐5, and Fe–Mo/HZSM‐5 catalysts in packed bed reactor

et al. 2019

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Summary A high abundance of methane and its relatively low price make it an attractive raw feedstock for the production of ethylene, which is in the consumer demand in recent years. Direct catalytic nonoxidative conversion is interesting, because it could be utilized on natural gas well sites. Monometallic and bimetallic Fe and Mo catalysts were prepared for the purpose of the coupling to ethane and ethene. Three supported materials were synthesized with the following loading of metal: 2.5‐wt% Fe, 5.0‐wt% Fe, and 2.5‐wt% Mo on HZSM‐5. Process' chemical reactions were also catalyzed with a constant 2.5‐wt% Mo/HZSM‐5, which had different amounts of Fe, namely, 0.5, 1.0, and 2.5 wt%. Fourier transform infrared (FTIR), N2 adsorption/desorption, NH3 temperature‐programmed desorption (TPD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X‐ray diffraction (XRD) were applied for characterization. Coke, accumulated on spent solids, was determined by thermogravimetric analysis (TGA). Activity was evaluated in quartz‐packed bed reactor. All surfaces suffered from deactivation due to carbon formation. The addition of Fe to Mo increased CH4 reacted. The highest selectivity for alkenes was achieved over 1.0‐wt% Fe to 2.5‐wt% Mo/HZSM‐5. At the peak of performance, the C‐based reactivity was 52% for olefins and 2% for alkanes. Stability was accomplished over 2.5‐wt% Fe/HZSM‐5, where the rate of C2 synthesis was comparatively stable for 20 hours of the time on stream. The selective C‐basis yield for C2H4 and C2H6 was 36% and 23%, respectively. The lowest measured quantity of (carbonaceous) by‐products was deposited on 2.5‐wt% Fe/HZSM‐5 after 26 hours. Propylene was detected very limitedly.

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Section: Resultsmentioning

confidence: 85%

Section: Resultsmentioning

confidence: 86%

Section: Resultsmentioning

confidence: 94%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Nonoxidative methane activation, coupling, and conversion to ethane, ethylene, and hydrogen over Fe/HZSM‐5, Mo/HZSM‐5, and Fe–Mo/HZSM‐5 catalysts in packed bed reactor

et al. 2019

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Frontiers in Arene Chemistry: Direct Methylation of Benzene with Methane on Metal‐Loaded Zeolites

Tsuji¹,

Katada

2023

Industrial Arene Chemistry

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Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

2020

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However, due to growing concerns regarding crude oil depletion and increasing environmental requirements, finding abundant fossil hydrocarbons with high H 2 /C ratios as well as alternative carbon resources has become crucial to maintaining sustainable, environmentally benign systems that can aid human development. [2] Thus, one-carbon (C1) chemistry, which is the chemistry of C1 molecules that can be derived from sources other than fossil hydrocarbons, including carbon monoxide (CO), carbon dioxide (CO 2), methane (CH 4), methanol (CH 3 OH), and formic acid (HCOOH), has emerged and plays important roles in the energy supply and high-value chemical preparation. [1,3] These C1 resources can be obtained from natural gas, shale gas, coal, biomass, solid wastes, and CO 2 emissions. [3a,4] Extensive studies have been dedicated to the catalytic conversion of C1 molecules, including production of dimethyl ether (DME) and liquid fuels from syngas (a mixture of CO and H 2); production of methanol, light olefins, and even aromatics from CH 4 ; and production of hydrogen from HCOOH. [5] All of these transformations require metallic catalytic species such as single atoms; clusters; or oxides, carbides, or alloy particles (e.g., Rh-, AuPd-, Fe 3 O 4-, and Fe 5 C 2-based catalysts). However, these isolated metallic species suffer from severe sintering due to a lack of confinement effects from supports, which leads to poor catalytic stability and decreased selectivities toward their target products. The efficient production of a specific range of hydrocarbons or oxygenates remains a difficult scientific and technical challenge. Overcoming product selectivity limitations and improving catalyst stabilities via catalyst designs are important areas of research. Zeolites are an important class of shape-selective catalysts with uniform micropores, tunable acidities, and high thermal and hydrothermal stabilities. Over the past decade, they have gained broad popularity and been applied to various industrially important catalytic processes. [6] In particular, the design and development of zeolite-based mono-, bi-, and multifunctional catalysts that combine the advantages of zeolites with those of metallic catalytic species have boosted the application of zeolites to C1 chemistry. As shown in Figure 1, value-added hydrocarbons and oxygenates can be produced from C1 molecules via various catalytic routes over zeolite-based catalysts. By May of 2020, the Structure Commission of the International C1 chemistry, which is the catalytic transformation of C1 molecules including CO, CO 2 , CH 4 , CH 3 OH, and HCOOH, plays an important role in providing energy and chemical supplies while meeting environmental requirements. Zeolites are highly efficient solid catalysts used in the chemical industry. The design and development of zeolite-based mono-, bi-, and multifunctional catalysts has led to a booming application of zeolite-based catalysts to C1 chemistry. Combining the advantages of zeolites and metallic catalytic species has promoted the catal...

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Active phase, catalytic activity, and induction period of Fe/zeolite material in nonoxidative aromatization of methane

Cited by 244 publications

References 39 publications

Nonoxidative methane activation, coupling, and conversion to ethane, ethylene, and hydrogen over Fe/HZSM‐5, Mo/HZSM‐5, and Fe–Mo/HZSM‐5 catalysts in packed bed reactor

Nonoxidative methane activation, coupling, and conversion to ethane, ethylene, and hydrogen over Fe/HZSM‐5, Mo/HZSM‐5, and Fe–Mo/HZSM‐5 catalysts in packed bed reactor

Frontiers in Arene Chemistry: Direct Methylation of Benzene with Methane on Metal‐Loaded Zeolites

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

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