DRIFT Studies for the Reaction and Adsorption of Alcohols and Isobutylene on Acidic Resin Catalysts and the Mechanism of ETBE and MTBE Synthesis

Doğu, Timur; Boz, and Nezahat; Aydin, Ebru; Oktar, Nuray; Murtezaoǧlu, and Kırali; Doğu, Gülşen

doi:10.1021/ie000922a

Cited by 34 publications

(19 citation statements)

References 18 publications

(48 reference statements)

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“…Kinetic studies reported in the literature10–15 and our recent DRIFT [diffuse reflectance FTIR (spectroscopy)] studies16 showed that a Langmuir–Hinshelwood‐type reaction mechanism, involving adsorbed alcohols and tert ‐olefins, gave good agreement with the kinetic data. However, Rideal–Eley‐type reaction mechanisms, involving fluid‐phase isoolefins and adsorbed alcohols in the rate‐determining step of the reaction, were also considered in a number of other studies 17–19.…”

Section: Introductionsupporting

confidence: 53%

“…There are a number of mechanisms, including Langmuir–Hinshelwood and Rideal–Eley‐type rate models, proposed in the literature for such etherification reactions 9, 10, 13, 17–19. From the DRIFT studies conducted in our previous work16 it was shown that adsorbed alcohols and adsorbed isoolefin molecules both participate in the reaction mechanism in vapor‐phase etherification reactions. However, the adsorption equilibrium constants of alcohols are much higher than the adsorption equilibrium constants of isoolefins.…”

Section: Resultsmentioning

confidence: 99%

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Reflux–recycle–reactor for high yield and selectivity in TAME and TAEE production

Boz

Doğu

2005

AIChE Journal

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Section: Introductionsupporting

confidence: 53%

Section: Resultsmentioning

confidence: 99%

Reflux–recycle–reactor for high yield and selectivity in TAME and TAEE production

Boz

Doğu

2005

AIChE Journal

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“…Thus loading the active sulfonic resin on the surface of a solid carrier facilitates the increased selectivity of the catalyst. The active centers in samples of this series of catalysts are uniform in structure and are acid sulfonic groups [14] which allows for the correlation of the catalytic activity of the sulfonic resins with the total acidity of the samples.…”

Section: Resultsmentioning

confidence: 99%

Catalytic characteristics of massive and loaded sulfonic resins in the synthesis of ethyl tert-butyl ether at atmospheric and increased pressure

et al. 2010

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The catalytic characteristics of massive and loaded sulfonic resins in the synthesis of ethyl tert-butyl ether at atmospheric and increased pressures have been compared. It has been established that massive sulfonic resins are more active than loaded resins at atmospheric pressure. At higher pressures, on the other hand, the activity and selectivity of catalysts are greater the lower the content of polymer as a result of the increased effectiveness of the acid centers.Recently alkyl tert-butyl ethers have been obtained industrially by the use of sulfonic resin catalysts of various types [1,2]. Structurally they may be gels or macroporous. The gel cation exchangers are deprived of porosity and most of their acid centers are used for adsorption (and consequently for catalytic reactions) only on swelling in polar media, while the macroporous catalysts have developed surfaces thanks to their porosity and their acid centers are available in both the swollen and unswollen states. The catalytic activity and selectivity of the organic sulfonic resins is determined by the presence of the sulfonic acid groups, located both on the surface and within the porous structure of the granules. The basic drawback of such materials is, in particular, the low mass-exchange characteristic, which is an important limitation to the use of massive sulfonic resins [3].To avoid the drawbacks of the massive sulfonic resins hybrid mineral-organic acid catalysts have been created, in which the organic sulfonic resin phase is distributed in the porous structure of the inorganic carrier (Al 2 O 3 , SiO 2 , zeolites, clays, ceramics, graphite). These catalysts, in contrast to ion exchange resins, are characterized by the rapid establishment of the adsorption equilibrium, which is not limited by internal diffusion.Mineral-organic sulfonic resins based on silica have been known for a long time and have been used as the basis of adsorption processes because of their high mass-exchange characteristics. Information on the use of such materials as catalysts is scattered, unsystematic and limited in character [4][5][6][7][8][9][10]. For example aluminosilicate with a loaded thermostable sulfonic

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“…One study reported that ethanol adsorbed from n-heptane onto a strong acid exchanger/catalyst (Amberlyst 15), with equilibrium binding constants reported to be in the range 10 1 -10 2 M -1 . 36 A second set of studies reported that phenols adsorbed from heptane and toluene onto tertiary amine sorbents via a hydrogenbonding mechanism. Binding constants for these studies were reported to be 10 0 -10 2 M -1 depending on the phenol.…”

Section: Results and Discusssionmentioning

confidence: 99%

Enhanced Hydrogen Bonding for the Adsorptive Recovery and Separations of Oxygenated Aromatic Compounds from Renewable Resources

Brown

Chen

Embree

et al. 2002

Ind. Eng. Chem. Res.

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Chemicals that are available from renewable resources typically contain heteroatoms that make hydrogen bonding a prominent intermolecular interaction. We are examining how hydrogen bonding can be exploited as an adsorption mechanism to facilitate the recovery and separations of oxygenated aromatic compounds from renewable resources. Specifically, we examined the adsorption of compounds that have weak or attenuated hydrogen-bonding abilities. The solvent in our study was hexane, which is commonly used in the food industry to extract chemicals from plant material (e.g., for vegetable oils and flavor extracts). The low dielectric constant of hexane also facilitates the hydrogen-bonding adsorption mechanism. Three polymeric adsorbents of differing basicities were studied, an acrylic ester sorbent (XAD-7, Rohm and Haas), a pyridine sorbent (Reillex 425, Reilly Industries), and a tertiary amine sorbent (IRA-93, Rohm and Haas). Adsorption affinities (related to the adsorption equilibrium constant, K eq ) and adsorption enthalpies (-∆H°) were observed to increase with increasing basicity of the sorbent's binding site. Infrared spectroscopy was used to study the interaction mechanism between the solutes and small-molecule analogues of the binding sites for the three sorbents. These studies support the conclusion that the observed increase in adsorption results from increased hydrogen-bond strengths. These results indicate that, by adjusting the hydrogen-bond accepting abilities of the adsorbent, it is possible to alter adsorption affinities to balance the dual objectives of recovery and selectivity.

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DRIFT Studies for the Reaction and Adsorption of Alcohols and Isobutylene on Acidic Resin Catalysts and the Mechanism of ETBE and MTBE Synthesis

Cited by 34 publications

References 18 publications

Reflux–recycle–reactor for high yield and selectivity in TAME and TAEE production

Reflux–recycle–reactor for high yield and selectivity in TAME and TAEE production

Catalytic characteristics of massive and loaded sulfonic resins in the synthesis of ethyl tert-butyl ether at atmospheric and increased pressure

Enhanced Hydrogen Bonding for the Adsorptive Recovery and Separations of Oxygenated Aromatic Compounds from Renewable Resources

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