Ethanol Conversion on MCM-41 and FSM-16, and on Ni-Doped MCM-41 and FSM-16 Prepared without Hydrothermal Conditions

Sugiyama, Shigeru; Kato, Yuhki; Wada, Takahiro; Ogawa, Shirou; Nakagawa, Keizo; Sotowa, Ken‐Ichiro

doi:10.1007/s11244-010-9485-9

Cited by 29 publications

(23 citation statements)

References 13 publications

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“…[8b] Indeed, this was confirmed by preliminary results from our group [9] and subsequently by Sugiyama et al [10] The pore diameters of M41 are usually 1.5-5.0 nm, and, therefore the product distribution on the catalysts is not controlled by shape selectivity. The reaction mechanism/pathways are of interest, and the target of our present study.…”

supporting

confidence: 60%

Conversion of Ethanol into Polyolefin Building Blocks: Reaction Pathways on Nickel Ion‐loaded Mesoporous Silica

2011

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The use of bioethanol (bEtOH) as an alternative (or additive) for automobile fuels has increased rapidly all over the world. This is one way of using renewable resources to suppress carbon dioxide emissions, while another challenge is the conversion of bEtOH to various olefins and their use for production of chemicals and polymers. [1][2][3][4][5][6][7] The latter would be very significant for the long-term fixation of carbon dioxide. Many efforts have therefore been devoted to the development of systems for converting bEtOH to ethene (C2 = ) and other lower olefins. In particular conversion to propene (C3 = ) is desirable due to the greater demand for C3= derivatives, such as propene oxide, acrylonitrile, and polypropene.[2]Catalytic conversions of EtOH on zeolites [3][4][5] and metal oxides [6, 7] have been widely studied. On zeolites, the activity and selectivity in the many studies reported so far are insufficient. The major weakness is catalyst deactivation. For example, the selectivity towards C3 = on proton-or metal-modified zeolites is usually ca. 20-30 % and decreases with reaction time, although sometimes higher C3 = selectivity values are observed upon catalyst degradation. [3][4][5] Oligomerization, polymerization, and fission reactions on strong acid sites in zeolite pores result in the formation of C3 = and butenes (C4 = ) due to shape selectivity. [3][4][5] However, the random reactions in the pores finally result in coke formation and short catalyst life times. EtOH can also react on metal oxide surfaces to give various chemicals. Acid sites are widely recognized to lead to dehydration of EtOH, giving C2 = , while basic sites lead to dehydrogenation to yield acetaldehyde (AA). [6, 7] As a result, many kinds of products, for example aldehydes, ketones, C2 [8] Therefore, Ni-M41 is a possible catalyst for the conversion of EtOH to C3 = since M41 is active for the dehydration of EtOH to yield C2 = .[8b] Indeed, this was confirmed by preliminary results from our group [9] and subsequently by Sugiyama et al.[10] The pore diameters of M41 are usually 1.5-5.0 nm, and, therefore the product distribution on the catalysts is not controlled by shape selectivity. The reaction mechanism/pathways are of interest, and the target of our present study.The influence of temperature on EtOH conversion over Ni-M41 is summarized in Figure 1. Many kinds of products were formed in addition to C2 = . Diethylether (DEE) was mainly obtained at around 523 K. DEE has been reported earlier as an intermediate compound in the dehydration, decomposing to yield EtOH and C2= at higher temperatures.[8b] The C2 = yield sharply increased at 573 K, and reached ca. 70 % at 623 K or above. The C4 = yield reached a maximum at 623 K, while maxima in C3 = yield occurred at 673 and 723 K. Notably, AA was formed at 573-723 K, although not in large amounts, which will be discussed later. The stability of Ni-M41 was examined at 673 K. As shown in Figure 2, the catalytic activity did not change during 20 h of continuous time on stream. In addi...

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confidence: 60%

Conversion of Ethanol into Polyolefin Building Blocks: Reaction Pathways on Nickel Ion‐loaded Mesoporous Silica

2011

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“…However, ethylene from ethanol can be obtained by different reaction mechanisms (Eqs. (1)- (3)) [Haishi et al, 2011;Makshina et al, 2012;Sugiyama et al, 2010]. Equation (1) seems to be the most favorable since, during ethanol conversion on Al-MCM-41, diethyl ether (C 2 H 5 OC 2 H 5 ) was never observed.…”

Section: Characterizationmentioning

confidence: 99%

“…Consequently, the discovery of the mesoporous silica molecular sieve (MCM-41) by the Mobil Oil Company resulted in considerable attention because of its uniform structure and pore size distribution. However, the pure silica MCM-41 has a neutral framework [Corma, 1997;Herbst et al, 1995;Kresge et al, 1992], which limits its industrial application due to its poor hydrothermal stability, low catalytic activity and weak surface acidity [Li et al, 2012;Sugiyama et al, 2010;Tuel, 1999] , Fe 3+ replace some of the silicon atoms in the walls of the mesoporous silica, the framework acquires a negative charge that can be compensated by protons, and the resulting solids can be used in acid catalysts [Tuel, 1999]. The Al-containing MCM-41 (Al-MCM-41) is one of the most studied MCM-41.…”

Section: Introductionmentioning

confidence: 99%

VAPOR-PHASE CATALYTIC CONVERSION OF ETHANOL INTO 1,3-BUTADIENE ON Cr-Ba/MCM-41 CATALYSTS

La-Salvia

Lovón-Quintana

Valença

2015

Braz. J. Chem. Eng.

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-Al-MCM-41, 16%Ba/Al-MCM-41 and 1.4%Cr-16%Ba/Al-MCM-41 were used as catalysts in the vapor-phase catalytic conversion of ethanol. Physical-chemical properties of the catalysts and the effect of barium and chromium on the Al-MCM-41 activity and 1,3-butadiene yield were studied. The catalysts were characterized by X-ray diffraction (XRD), N 2 physisorption (BET method), CO 2 chemisorption and Fourier transform infrared spectroscopy (FT-IR). When ethanol was completely converted on Al-MCM-41 and 16%Ba/Al-MCM-41, the reaction products showed a high selectivity for ethylene (90-98%). However, on the 1.4%Cr-16%Ba/Al-MCM-41 catalyst, a greater number of reaction products were obtained such as ethylene, acetaldehyde, diethyl ether and 1,3-butadiene. The maximum 1,3-butadiene yield obtained from ethanol reaction was 25% at 723 K and W/F EtOH = 15 g h mol -1 . The latter result was obtained in a single step and without addition of reaction promoters (e.g., acetaldehyde, crotonaldehyde, hydrogen) in the feed stream to the reactor.

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“…8) Furthermore, Ni 2+ was incorporated into FSM-16 via the TIE procedure, and the resultant solid showed great catalytic activity in a conversion of ethanol to propylene. 10) In the TIE procedure, mesoporous silica such as MCM-41 or FSM-16 was not directly used, while a precursor of mesoporous silica (as-synthesized MCM-41 or FSM-16), a dried solid mixture consisting of a silica-source and a template surfactant, was used for the ion exchange with various cations. This demonstrated that the TIE procedure for the incorporation of various cations into mesoporous silica is a unique preparation procedure for an active catalyst.…”

Section: Introductionmentioning

confidence: 99%

Effect of the template ion exchange behaviors of chromium into FSM-16 on the oxidative dehydrogenation of isobutane

Ehiro

Itagaki

Kurashina

et al. 2015

J. Ceram. Soc. Japan

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The template ion exchange of chromium cations into FSM-16 (#16 Folded Sheets Mesoporous Materials) for 247 h resulted in a 2.89 wt % incorporation of those cations into the FSM-16, although only a 0.3 wt % incorporation had previously been reported. The XRD pattern of the resultant solid (Cr-FSM-16) showed that the hexagonal structure characteristic of FSM-16 remained after the 2.89 wt % incorporation of chromium cations. XPS could be used to detect the Cr 3+ and Cr 6+ species on the surface of Cr-FSM-16. A pre-edge peak that was due to a tetrahedrally coordinated Cr 6+ species was confirmed in the XANES spectrum of the Cr-FSM-16, which showed that the coordination state around some Cr species was similar to that around the Si species in FSM-16. With the increase in the amount of chromium cations in FSM-16, its catalytic activity and stability during the oxidative dehydrogenation of isobutane were evidently improved.

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Ethanol Conversion on MCM-41 and FSM-16, and on Ni-Doped MCM-41 and FSM-16 Prepared without Hydrothermal Conditions

Cited by 29 publications

References 13 publications

Conversion of Ethanol into Polyolefin Building Blocks: Reaction Pathways on Nickel Ion‐loaded Mesoporous Silica

Conversion of Ethanol into Polyolefin Building Blocks: Reaction Pathways on Nickel Ion‐loaded Mesoporous Silica

VAPOR-PHASE CATALYTIC CONVERSION OF ETHANOL INTO 1,3-BUTADIENE ON Cr-Ba/MCM-41 CATALYSTS

Effect of the template ion exchange behaviors of chromium into FSM-16 on the oxidative dehydrogenation of isobutane

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