Direct conversion of methane on Mo/ZSM-5 catalysts to produce benzene and hydrogen: achievements and perspectives

Ismagilov, Z. R.; Матус, Е. В.; Цикоза, Л. Т.

doi:10.1039/b810981h

Cited by 235 publications

(179 citation statements)

References 168 publications

(418 reference statements)

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“…summarized by the term 'methane aromatization' (MA). Details on this reaction can be found in reviews by Ismagilov [105], Bao [106] or Spivey and Hutchings [107]. A thermodynamic analysis of methane aromatization with and without coke removing agents like H 2 O, CO and CO 2 can be found in Ref.…”

Section: Methane Aromatizationmentioning

confidence: 99%

Methane Activation by Heterogeneous Catalysis

2014

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Methane activation by heterogeneous catalysis will play a key role to secure the supply of energy, chemicals and fuels in the future. Methane is the main constituent of natural gas and biogas and it is also found in crystalline hydrates at the continental slopes of many oceans and in permafrost areas. In view of this vast reserves and resources, the use of methane as chemical feedstock has to be intensified. The present review presents recent results and developments in heterogeneous catalytic methane conversion to synthesis gas, hydrogen cyanide, ethylene, methanol, formaldehyde, methyl chloride, methyl bromide and aromatics. After presenting recent estimates of methane reserves and resources the physico-chemical challenges of methane activation are discussed. Subsequent to this recent results in methane conversion to synthesis gas by steam reforming, dry reforming, autothermal reforming and catalytic partial oxidation are presented. The high temperature methane conversion to hydrogen cyanide via the BMA-process and the Andrussow-process is considered as well. The second part of this review focuses on one-step conversion of methane into chemicals. This includes the oxidative coupling of methane to ethylene mediated by oxygen and sulfur, the direct oxidation of methane to formaldehyde and methanol, the halogenation and oxyhalogenation of methane to methyl chloride and methyl bromide and finally the non-oxidative methane aromatization to benzene and related aromates. Opportunities and limits of the various activation strategies are discussed.

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Section: Methane Aromatizationmentioning

confidence: 99%

Methane Activation by Heterogeneous Catalysis

2014

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“…Both thermodynamic and kinetic constraints cause methane conversion in MDA process to remain low level [147]. Methane conversion can be enhanced by increasing the reaction temperature or decreasing the reaction pressure, neither of which may be favorable or suitable for further industrial development.…”

Section: Membrane Reactorsmentioning

confidence: 99%

Recent progress in methane dehydroaromatization: From laboratory curiosities to promising technology

Guo

Zhao

et al. 2013

Journal of Energy Chemistry

227

183

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“…H2 is formed as a valuable by-product, and its selective removal from the reaction medium may improve the process by shifting the equilibrium controlled reaction. Moreover, the use of the adequate shape-selective catalyst under optimized process conditions may maximize the selectivity to aromatics 10,11 .…”

Section: Introductionmentioning

confidence: 99%

“…Regarding the possible zeolites, the most adequate are those with structures containing pores of dimensions close to the dynamic diameter of benzene, the desired product9. Thus, ZSM-5 11,15,16 and MCM-22 11,[17][18][19][20][21] have been thoroughly studied, although other zeolite structures presenting 10-ring channels , such as IM-5 22,23 or TNU-9 24 , have also been recently described for this process. Regarding the reaction mechanism and the active sites involved, it is widely accepted that methane is first activated on the Mo sites and the reaction intermediates formed will further oligomerize, cyclate and dehydrogenate on the Brønsted acid sites.…”

Section: Introductionmentioning

confidence: 99%

Non-oxidative dehydroaromatization of methane: an effective reaction–regeneration cyclic operation for catalyst life extension

Portilla

Llopis²,

Martı́nez

2015

Catal. Sci. Technol.

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Non-oxidative methane aromatization is an attractive direct route for producing higher hydrocarbons, highly selective to benzene despite the low conversions due to thermodynamic limitations, and Mo/H-ZSM-5, the first catalyst proposed for this reaction, is still considered as one of the most adequate. The major problem of this process is the severe catalyst deactivation due to the rapid buildup of carbonaceous deposits on the catalysts.Here we present an effective regeneration procedure that extends the life of Mo/zeolite based catalysts by combining reaction periods of 1.5 h with 0.5 h regeneration steps in a continuous cyclic mode and methane activation after each regeneration stage. Benzene productivity obtained with Mo/ZSM-5 is shown to be almost constant for increasing TOS ranges when applying this new cyclic protocol, and threefold values are achieved for an 18 h on stream period by limiting the reaction steps to the first 1.5 h of maximum benzene selectivity (97 vs. 33 g benzene/kg cat·h) as compared to a conventional single run.

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Direct conversion of methane on Mo/ZSM-5 catalysts to produce benzene and hydrogen: achievements and perspectives

Cited by 235 publications

References 168 publications

Methane Activation by Heterogeneous Catalysis

Methane Activation by Heterogeneous Catalysis

Recent progress in methane dehydroaromatization: From laboratory curiosities to promising technology

Non-oxidative dehydroaromatization of methane: an effective reaction–regeneration cyclic operation for catalyst life extension

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