Natural gas conversion to liquid fuels in a zone reactor

Breed, A.W.; Doherty, Michael F.; Gadewar, Sagar B.; Grosso, Phil; Lorković, Ivan M.; McFarland, Eric W.; Weiss, Michael J.

doi:10.1016/j.cattod.2005.08.001

Cited by 40 publications

(29 citation statements)

References 3 publications

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“…Svelle et al berichten über einen mittels Propenpuls voraktivierten H-SAPO-34-Katalysator, bei dem bei 350 8C der anfängliche Methanolumsatz um das 25-fache hçher lag als der Umsatz für Methylchlorid oder Methylbromid bei gleichen Bedingungen. [194][195][196][197] In diesem integrierten Prozess beobachteten sie eine schnellere Deak- 761 kJ mol À1 [190] ), [191,192] was ferner durch Ergebnisse der Coreaktion von 13 C-markiertem Methylchlorid mit Ethen und Propen gestützt wurde.…”

Section: Methylhalogenideunclassified

Umwandlung von Methanol in Kohlenwasserstoffe: Wie Zeolith‐Hohlräume und Porengröße die Produktselektivität bestimmen

et al. 2012

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Flüssige Kohlenwasserstoffe nehmen aufgrund ihrer hohen Energiedichte und guten Transportfähigkeit eine Schlüsselrolle in der globalen Energieversorgung ein. Eine vergleichbare Bedeutung haben niedere Alkene wie Ethylen und Propylen in der Produktion von Verbrauchsgütern. In einer Gesellschaft der Nach‐Erdöl‐Zeit wird die Produktion von Kraftstoffen und Alkenen auf alternative Quellen wie Biomasse, Kohle, Erdgas und CO2 angewiesen sein. Die Umwandlung von Methanol in Kohlenwasserstoffe, bekannt als Methanol‐to‐ Hydrocarbons(MTH)‐Reaktion, könnte eine zentrale Rolle auf diesem Weg einnehmen, weil je nach Wahl des Katalysators und der Reaktionsbedingungen gezielt Benzin (Methanol‐to‐Gasoline, MTG) oder Alkene (Methanol‐to‐Olefins, MTO) hergestellt werden können. Dieser Aufsatz beschreibt eine Reihe von industriellen MTH‐Projekten, die in den letzten Jahren realisiert wurden, sowie den aktuellen Stand der Grundlagenforschung zur Synthese und Anwendung von mikroporösen Materialien für die gezielte Veränderung von Selektivität und Lebensdauer der Katalysatoren.

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Section: Methylhalogenideunclassified

Umwandlung von Methanol in Kohlenwasserstoffe: Wie Zeolith‐Hohlräume und Porengröße die Produktselektivität bestimmen

et al. 2012

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“…The studies by Ford et al and the present article show that methyl bromide may readily be converted into higher hydrocarbons at fairly low temperatures around 350-400 8C or 160-210 8C, respectively. High single-pass conversions of 70 % methane [37] or 60-80 mol % methyl bromide can yield C2-C6 or C2-C5 hydrocarbons, respectively (see flow diagram in Figure 9). Only small amounts of CH 3 Br are converted back into methane and may be recycled.…”

Section: àmentioning

confidence: 99%

“…methylene equivalents (e.g., MeX = CH 2 + HX; MeÀX with X = OH, Cl, Br) [12,20,31,[37][38][39][41][42][43][44][45] generally relies on the use of zeolites or solid acids as oxide-based catalysts. While they work quite well with methanol, [20,29] methyl bromide is highly corrosive and is likely to enable chemical transport of many oxides, thus destroying any oxide-based catalyst during prolonged use.…”

Section: Introductionmentioning

confidence: 99%

Direct Coupling of Bromine‐Mediated Methane Activation and Carbon‐Deposit Gasification

Osterwalder¹,

Stark²

2007

ChemPhysChem

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The direct bromination of methane offers a quite selective (>98 %) route towards methane activation but shifts the problem of fuel production to converting and handling corrosive methyl bromide. The direct conversion of methyl bromide, at about 200 degrees C, into light hydrocarbons can be catalyzed under pressure by AlBr(3) resulting in the formation of propane-rich mixtures of light hydrocarbons, carbonaceous deposits, and HBr. After releasing the gaseous products, the addition of hydrogen at 260 degrees C allows a quantitative conversion of the carbonaceous deposits into the same range of light hydrocarbons. These second-stage products efficiently contribute to the overall process yield while enabling a full regeneration of the catalyst's activity. This oxygen-free process is compared to the conversion of methyl bromide on zeolites and the currently used methanol-to-gasoline (MTG) process in terms of product distributions and apparent energy of activation. A detailed chemical analysis of the intermediates revealed the presence of a carbon pool consisting of highly substituted benzene and cyclopentadiene derivatives, as observed on zeolites used in the MTG process. This similarity suggests that the currently used oxygen-based syngas/MTG process for methane conversion may be extended to a bromine-mediated process by using methyl bromide as an intermediate instead of methanol.

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“…Modifications to the process employing oxybromination have faced similar challenges [13][14][15][16]. A continuous process approach to separation of HBr, and regeneration of bromine using a regenerable solid metal oxide in a switched-bed zone reactor, has been proposed [17]. Unfortunately, the large lattice size change associated with the solid oxide-to-bromide cycle limits lifetime, cycleablility, and the regenerable bromine capacity of the solid reactants.…”

Section: Introductionmentioning

confidence: 99%

Molten salt chemical looping for reactive separation of HBr in a halogen-based natural gas conversion process

Upham

Snodgrass

Zavareh

et al. 2017

Chemical Engineering Science

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Hydrogen bromide (HBr) oxidation to molecular bromine (Br 2 ) is demonstrated in a chemical looping process using a molten bromide salt. The two-step process is operated at 500 °C and first contacts oxygen with molten KBr-LiBr-NiBr 2 to form Br 2 gas and a suspension of nickel oxide (NiO) particles in one reactor. The oxide suspension is then contacted with HBr to regenerate the bromide salt and produce steam. Sixty-eight metal oxides/bromides were considered. The cyclic interconversion between oxide and bromide, by alternating exposure to HBr and oxygen, at a single temperature was only possible with nickel. In contrast to solidbased chemical looping systems, the liquid bromide salt (NiBr 2 dissolved in KBr-LiBr eutectic) was found to be cycleable without attrition or deactivation. Further, when mixtures of olefins and hydrogen bromide were reacted with the oxide suspension, selective oxidation of HBr was observed without hydrocarbon oxidation. High selectivity for HBr oxidation is due to the solubility of HBr in the molten salt, which allows contact with NiO, whereas, the insoluble hydrocarbons do not contact the reactive oxide. A process model that makes use of reactive separation of HBr from hydrocarbons and process intensification using molten salt-based chemical looping is presented as a potentially lower cost alternative to a process model using conventional separations in bromine-based methane conversion. The total heat exchanged in a corrosive environment in the molten salt based process is 205 MW, and the heat exchanged in a corrosive environment in the conventional process is 581 MW.

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Natural gas conversion to liquid fuels in a zone reactor

Cited by 40 publications

References 3 publications

Umwandlung von Methanol in Kohlenwasserstoffe: Wie Zeolith‐Hohlräume und Porengröße die Produktselektivität bestimmen

Umwandlung von Methanol in Kohlenwasserstoffe: Wie Zeolith‐Hohlräume und Porengröße die Produktselektivität bestimmen

Direct Coupling of Bromine‐Mediated Methane Activation and Carbon‐Deposit Gasification

Molten salt chemical looping for reactive separation of HBr in a halogen-based natural gas conversion process

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