Catalysis Chemistry of Dimethyl Ether Synthesis

Sun, Jian; Yang, Guohui; Yoneyama, Yoshiharu; Tsubaki, Noritatsu

doi:10.1021/cs500967j

Cited by 260 publications

(228 citation statements)

References 119 publications

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“…From this data, it was expected that these acidic WO 3 catalysts would be beneficial in the selective dehydration of methanol to dimethyl ether. 14,15,41 Importantly, Au NPs did not affect the acidity of the WO 3 -containing catalysts, as determined by NH 3 -TPD. During methanol transformation catalysis, however, Au NPs influenced the activity and selectivity of the WO 3 catalysts, which is discussed below.…”

Section: Resultsmentioning

confidence: 94%

“…The MeOH dehydration reaction to yield DME is very appealing due to the potential widespread use of DME as an alternative fuel to help meet our future energy needs. [15][16][17][18] Industrially, this reaction is usually carried out over γ-Al 2 O 3 or zeolites such as ZSM-5, 19,20 which possess strong acid sites that are prone to rapid deactivation. Weaker acid sites on WO 3 are expected to have lower rates of deactivation at the expense of lower activities compared to these industrial catalysts.…”

Section: Introductionmentioning

confidence: 99%

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Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

et al. 2016

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American Chemical SocietyDepuccio, DP.; Ruiz-Rodríguez, L.; Rodriguez-Castellon, E.; Botella Asuncion, P.; López Nieto, JM.; Landry, CC. (2016) AbstractAnalyzing the structural and chemical properties of materials at the interface of metal nanoparticles and metal oxide supports is important for catalytic applications. Tungsten oxide (WO 3 ) is a widely studied catalyst, but changing the catalytic reactivity at the surface of this oxide with metal nanoparticles is of interest. In this work, we sought to modify the redox properties of porous WO 3 and SiO 2 -WO 3 catalysts with sonochemically deposited gold nanoparticles (Au NPs) in order to access and study this reaction pathway. Characterization using powder X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), and inductively-coupled plasma optical emission spectroscopy (ICP-OES) confirmed that crystalline Au NPs with diameters of 5 -12 nm were distributed throughout the catalysts. Temperature-programmed desorption (TPD) was used to probe the surface acidity of the catalysts. The physic-chemical characteristics of catalysts have been also discussed by considering the catalytic performance of these materials in the aerobic transformation of methanol. Catalysts containing nanocrystalline WO 3 but no Au NPs displayed very high selectivity to DME (> 60%) at all conversions with minor oxidation reactivity, which highlighted the acidic nature of these catalysts. No effect on the acidity of the catalysts was observed by TPD when Au NPs were loaded in the catalysts. The reducibility of the crystalline WO 3 species, however, increased significantly due to the interaction with Au NPs, as observed by temperature-programmed reduction (TPR). In the gas-phase transformation of MeOH under aerobic conditions, catalysts modified with Au NPs showed greater activity compared to non-modified catalysts. In addition, oxidation selectivity to products such as methyl formate as well as formaldehyde, dimethoxymethane, and carbon oxides became heavily favored with only minor dehydration selectivity. The redox properties of these WO 3 catalysts could be tuned by changing the Au loading. More labile lattice oxygen and enhanced redox properties at the surface of WO 3 modified with Au NPs clearly altered these traditional dehydration catalysts to potential oxidation catalysts. Thus, modification of WO 3 with Au is an effective way to expand the MeOH transformation product distribution beyond DME to other useful, oxidized products not typically observed over pure WO 3 .

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Section: Resultsmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

et al. 2016

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“…While syngas conversion to methanol is significantly limited by equilibrium, further conversion of methanol to DME shifts the equilibrium toward more methanol formation and allows higher single-pass conversion. Hence, the direct DME synthesis is thermodynamically and economically more favorable than the two-step process [4,6,7].…”

Section: Introductionmentioning

confidence: 99%

Direct dimethyl ether synthesis from synthesis gas: The influence of methanol dehydration on methanol synthesis reaction

et al. 2016

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Direct dimethyl ether (DME) synthesis from synthesis gas is studied with regard to potential effects of methanol dehydration on methanol formation and copperbased catalyst performance. For this, the influence of the operating conditions (space velocity, temperature, pressure, time-on-stream and syngas composition) on activity, selectivity and stability of the catalyst was studied and compared for methanol synthesis and direct DME synthesis. The advantage of the direct over the two-step DME synthesis is apparent at conditions where syngas conversion to methanol is thermodynamically limited. However, under the applied operating conditions, results suggest that combining methanol synthesis and dehydration has a negative effect on the methanol formation kinetics. The origin of the observed phenomena is investigated by varying dehydration catalyst and by introducing dehydration products (DME and water) into the methanol synthesis feed. Choice of the solid acid catalyst does not seem to affect methanol formation, and DME is also found to be practically inert over the methanol synthesis catalysts. Water injection, on the other hand, led to a significant decrease in the methanol synthesis rate. Thus, formation of an additional amount of water through methanol dehydration might be an explanation for the lower methanol formation rate in the direct DME synthesis.

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“…1 3 particles are located on the surface, as revealed by the XPS results, they still may partially block the HZSM-5 microchannels and reduce the accessibility of micropores (Table 1). Moreover, the mesoporous volume of W/HZSM-5 increases first and then decreases with increasing W loading.…”

Section: Xrd and Textural Characterizationmentioning

confidence: 99%

“…At present, some catalytic conversion reactions of DME have been explored and progress has been achieved. Generally, the DME molecule can be easily activated to form CH 3 -, CH 3 O-and CH 3 OCH 2 -groups. Then the active groups can form hydrocarbons, like olefins, gasoline and aromatics, [5][6][7] through the hydrocarbon pool (HP) mechanism, or they can form oxygenated compounds such as methyl acetate, 8 formaldehyde (FA), 9 dimethoxymethane (DMM), 10,11 methyl formate (MF), 12 and ethanol.…”

Section: Introductionmentioning

confidence: 99%

Conversion of dimethyl ether to toluene under an O₂ stream over W/HZSM-5 catalysts

Wang

Liu

et al. 2015

Catal. Sci. Technol.

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The direct conversion of dimethyl ether (DME) to toluene without other aromatics is realized over W/HZSM-5 catalysts with high W contents. The influence of W content on the nature of tungsten species, the distribution of acid sites, the redox properties, and the subsequent catalytic performance of W/HZSM-5 in DME conversion was investigated. The introduction of a high content of W in HZSM-5 can bring about some new redox sites and acidic sites associated with W species, although they also cover some acidic sites in HZSM-5. In this way, the introduction of W interrupts the dual cycle of the DME-to-hydrocarbon reaction on HZSM-5, and effectively the formation of higher methylbenzenes is limited.

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Catalysis Chemistry of Dimethyl Ether Synthesis

Cited by 260 publications

References 119 publications

Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

Direct dimethyl ether synthesis from synthesis gas: The influence of methanol dehydration on methanol synthesis reaction

Conversion of dimethyl ether to toluene under an O₂ stream over W/HZSM-5 catalysts

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Catalysis Chemistry of Dimethyl Ether Synthesis

Cited by 260 publications

References 119 publications

Investigating the Influence of Au Nanoparticles on Porous SiO2–WO3 and WO3 Methanol Transformation Catalysts

Investigating the Influence of Au Nanoparticles on Porous SiO2–WO3 and WO3 Methanol Transformation Catalysts

Direct dimethyl ether synthesis from synthesis gas: The influence of methanol dehydration on methanol synthesis reaction

Conversion of dimethyl ether to toluene under an O2 stream over W/HZSM-5 catalysts

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Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

Investigating the Influence of Au Nanoparticles on Porous SiO₂–WO₃ and WO₃ Methanol Transformation Catalysts

Conversion of dimethyl ether to toluene under an O₂ stream over W/HZSM-5 catalysts