Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using physical mixtures of a commercial Cu/Zn/Al2O3 catalyst and several solid–acid catalysts

Semelsberger, Troy A.; Ott, Kevin C.; Borup, Rodney L.; Greene, Howard L.

doi:10.1016/j.apcatb.2006.02.015

Cited by 103 publications

(49 citation statements)

References 39 publications

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“…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%

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: 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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“…The hydrogen-type Zeolite Socony Mobil-5 (HZSM-5) has also been used as a support in the catalytic cracking of hydrocarbons and in a dimethyl ether reforming process. Its high efficiency in the dehydrogenation and rupture of C-C bonds has been reported by many researchers (Kawabata et al 2006;Semelsberger et al 2006). However, to our knowledge, there are few reports on bio-oil steam reforming over zeolites, in particular, HZSM-5.…”

Section: Introductionmentioning

confidence: 97%

Hydrogen Production via Acetic Acid Steam Reforming over HZSM-5 and Pd/HZSM-5 Catalysts and Subsequent Mechanism Studies

Wang

et al. 2013

BioResources

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Acetic acid (HOAc) was selected as a bio-oil model compound for the steam reforming of bio-oil for hydrogen production. The influence of temperature and steam-to-carbon ratio (S/C) on the steam reforming of HOAc over hydrogen-type Zeolite Socony Mobil-5 (HZSM-5) and the catalyst with added Pd (Pd/HZSM-5) have been investigated in a fixedbed reactor. Brunauer-Emmett-Teller surface area measurements, scanning electron microscopy, and transmission electron microscopy were performed to characterize the texture and structure of the catalysts. Upon addition of Pd to HZSM-5, the selectivity of the products was modified and the H 2 yield was greatly increased. The hydrogen yield and potential hydrogen yield from the steam reforming of HOAc were as high as 60.2% and 87.5%, respectively, under optimized reaction conditions. Both the conversion of HOAc and the H 2 yield over Pd/HZSM-5 were significantly enhanced with increasing S/C ratio and reaction temperature below 600 C, whereas the H 2 yield did not significantly increase at temperatures above 600 C. The mechanism of HOAc decomposition on the Pd(111) surface was calculated via density functional theory. The optimal decomposition route was found to be CH

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“…Even though methanol SR was easily performed at low temperature, methanol is not only biologically toxic in nature but also incompatible with the developed infrastructure especially for automobiles. In this regard, SR of dimethyl ether (DME) becomes one of the recent research interests (Takeishi and Suzuki, 2004;Tanaka et al, 2005;Faungnawakij et al, 2006;Kawabata et al, 2006;Semelsberger et al, 2006). DME can be reformed to hydrogen at low temperature, easily handled, and stored due to similar physical properties to liquefied petroleum gases (LPG).…”

Section: Introductionmentioning

confidence: 99%

“…Due to the endothermicity of RWGS, a lower reaction temperature is favored for lower CO selectivity. Although many efforts (Faungnawakij et al, 2006;Kawabata et al, 2006;Semelsberger et al, 2006) have been made to control the acidity of hybrid catalysts, it is desirable to continue more systematic study about the solid acids for better production of hydrogen especially at lower temperature.…”

Section: Introductionmentioning

confidence: 99%

Acidity Control of Al-SBA-15 and Its Effect on the Catalytic Performance for Steam Reforming of Dimethyl Ether

Yun

Bazardorj

Ihm

2009

J. Chem. Eng. Japan

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Steam reforming (SR) of dimethyl ether (DME) seems to proceed via a successive two step mechanism: hydrolysis of DME over solid acid catalysts, followed by methanol SR over copper-based catalysts. Since the DME hydrolysis is rate-controlling, it is desirable to continue more systematic study concerning the solid acids for better production of hydrogen. In this work, the composites of mesoporous solid acid catalysts (Al-SBA-15) and copper-based catalysts (Cu/ZnO/Al 2 O 3 ) made the hybrid catalysts, and they were used for DME SR. Acidity of Al-SBA-15 was controlled by tuning Si/Al ratio, which should vary the number of acidic sites. The reducibility of hybrid catalysts was varied with different weight ratio between Al-SBA-15 and Cu/ZnO/Al 2 O 3 . The catalytic activity of DME SR was analyzed in terms of acid amount and copper reducibility.

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Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using physical mixtures of a commercial Cu/Zn/Al2O3 catalyst and several solid–acid catalysts

Cited by 103 publications

References 39 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

Hydrogen Production via Acetic Acid Steam Reforming over HZSM-5 and Pd/HZSM-5 Catalysts and Subsequent Mechanism Studies

Acidity Control of Al-SBA-15 and Its Effect on the Catalytic Performance for Steam Reforming of Dimethyl Ether

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Generating hydrogen-rich fuel-cell feeds from dimethyl ether (DME) using physical mixtures of a commercial Cu/Zn/Al2O3 catalyst and several solid–acid catalysts

Cited by 103 publications

References 39 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

Hydrogen Production via Acetic Acid Steam Reforming over HZSM-5 and Pd/HZSM-5 Catalysts and Subsequent Mechanism Studies

Acidity Control of Al-SBA-15 and Its Effect on the Catalytic Performance for Steam Reforming of Dimethyl Ether

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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