The role of acid sites induced by defects in the etherification of HMF on Silicalite-1 catalysts

Lanzafame, Paola; Barbera, Katia; Perathoner, Siglinda; Centi, Gabriele; Aloise, A.; Migliori, Massimo; Macario, Anastasia; Nagy, J.B.; Giordano, G.

doi:10.1016/j.jcat.2015.07.028

Cited by 79 publications

(55 citation statements)

References 62 publications

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“…Moreover, DME can be produced from biomass or CO 2 and, as it can also be used as an intermediate to produce olefins and chemicals, it is considered a promising energetic vector of the future for introducing renewable energy in the chemical industry [9][10][11]. e valorisation of biomass by using zeolites is receiving a growing attention because it opens new ways for application of these materials in low temperature and liquid phase reactions of biomass or biomass-derived compounds [12,13]. Compared with other zeolites such as MFI, BEA, EUO, MTW, the 2-D small/medium pore system of FER-type zeolite inhibits the coke formation and offers high DME selectivity during methanol dehydration reaction [14,15].…”

Section: Introductionmentioning

confidence: 99%

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Catizzone

Migliori

Aloise

et al. 2019

Journal of Chemistry

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In contrast to high silica zeolites, it is difficult to obtain mesoporosity in zeolites with low Si/Al ratio (e.g., <20) via conventional NaOH-based treatment, making the obtainment of hierarchical zeolites with high acidity a challenging target. In this paper, we report the preparation of hierarchical FER-type zeolite at low Si/Al molar ratio (about 10) by postsynthesis etching involving a sequence of three treatments with NaAlO 2 , HCl, and NaOH solutions and investigate the effect of both NaAlO 2 solution concentration and time of treatment on the textural properties. e obtained materials exhibit a mesoporous volume higher than the parent ferrierite with no significant effect on the sample acidity. e catalytic activity of some samples was investigated in vapour-phase methanol dehydration to dimethyl ether, revealing the superiority of hierarchical zeolites in terms of methanol conversion, although the presence of mesopores causes formation of light hydrocarbons at high temperatures.

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Section: Introductionmentioning

confidence: 99%

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Catizzone

Migliori

Aloise

et al. 2019

Journal of Chemistry

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“…The B acid site density ( A B ) of the SO 4 2− /ZrO 2 ‐PMO‐SO 3 H was determined by titrating with dilute NaOH solution, whereas the L acid site density ( A L ) was calculated based on the n B / n L value . As summarized in Table , both B, and L acid site densities of three ordered mesoporous SO 4 2− /ZrO 2 ‐PMO‐SO 3 H catalysts decreased gradually with increasing Si/Zr molar ratios from 0.5, 1.0 to 2.0, owing to the gradually decreased proportion of the SO 4 2− /ZrO 2 units in the catalysts.…”

Section: Resultsmentioning

confidence: 99%

“…L, and B acid sites were quantified by integrating the area underneath the bands at 1450, and 1540 cm −1 , respectively,, the corresponding molar ratio of B‐to‐L acid was then estimated.…”

Section: Methodsmentioning

confidence: 99%

Design of Ordered Mesoporous Sulfonic Acid Functionalized ZrO₂/organosilica Bifunctional Catalysts for Direct Catalytic Conversion of Glucose to Ethyl Levulinate

et al. 2018

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Ordered mesoporous sulfonic acid functionalized ZrO 2 /organosilica catalysts (SO 4 2À /ZrO 2 -PMO-SO 3 H) bearing tunable Brønsted, and Lewis acid site distributions were prepared by a P123directed sol-gel co-condensation route followed by ClSO 3 H functionalization. As-prepared catalysts were applied in the conversion of glucose to ethyl levulinate in ethanol medium. The SO 4 2À /ZrO 2 -PMO-SO 3 H-catalyzed target reaction followed a glucose-ethyl glucoside-ethyl fructoside-5-ethoxymethylfurfuralethyl levulinate pathway dominated by the synergistic effect of the super strong Brønsted acidity, and moderate Lewis acidity of the catalysts. Additionally, by combining the advantages of the considerably high Brønsted (696 meq g À1 ), Lewis acid site density (703 meq g À1 ), optimal Brønsted/Lewis molar ratio (0.99), and excellent porosity properties, the SO 4 2À /ZrO 2 -PMO-SO 3 H1.0 obtained at an initial Si/Zr molar ratio of 1.0 exhibited the highest ethyl levulinate yield (42.3 %) among the various tested catalysts. Moreover, the SO 4 2À /ZrO 2 -PMO-SO 3 H can be reused three times without obvious changes in activity, morphology, and chemical structure.[a] Dr.

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“…Silicalite‐1 is an aluminum‐free crystalline zeolite with MFI topological framework. The presence of Si atom defective sites in their lattice can impose the formation of acid centers (silanol groups), which have been reported as active catalysts for the Beckmann rearrangement as well as the etherification of 5‐hydroxymethyl‐2‐furfural . More recently, we have found that the ZnO catalyst supported on Silicalite‐1 zeolite exhibits a superior catalytic performance for CO 2 assisted dehydrogenation of isobutane, which is far more active than SBA‐15‐supported one with the same Zn content .…”

Section: Background and Originality Contentmentioning

confidence: 92%

Isobutane Dehydrogenation Assisted by CO₂ over Silicalite‐1‐Supported ZnO Catalysts: Influence of Support Crystallite Size

et al. 2020

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Summary of main observation and conclusion The ZnO catalysts supported on Silicalite‐1 zeolites with different crystallite sizes (0.08, 0.35, 1 and 1.7 μm, respectively) and 5% Zn were synthesized via an incipient wetness method. The catalysts were characterized by XRD, N2 adsorption, SEM, TEM‐EDX, DRIFT spectra and NH3‐TPD, and their catalytic performance in isobutane dehydrogenation assisted by CO2 was investigated. The catalytic activity is strongly dependent on the crystallite size of Silicalite‐1 support. The ZnO/S‐1‐0.35 catalyst with ca. 0.35 μm crystallite size displays the highest activity, affording an initial isobutane conversion of 51.0% and 74.5% isobutene selectivity. This can be attributed to a higher amount of acid sites present on this catalyst as well as the largest amount of nest silanols possessed by the S‐1‐0.35 support.

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The role of acid sites induced by defects in the etherification of HMF on Silicalite-1 catalysts

Cited by 79 publications

References 62 publications

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Design of Ordered Mesoporous Sulfonic Acid Functionalized ZrO₂/organosilica Bifunctional Catalysts for Direct Catalytic Conversion of Glucose to Ethyl Levulinate

Isobutane Dehydrogenation Assisted by CO₂ over Silicalite‐1‐Supported ZnO Catalysts: Influence of Support Crystallite Size

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The role of acid sites induced by defects in the etherification of HMF on Silicalite-1 catalysts

Cited by 79 publications

References 62 publications

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Hierarchical Low Si/Al Ratio Ferrierite Zeolite by Sequential Postsynthesis Treatment: Catalytic Assessment in Dehydration Reaction of Methanol

Design of Ordered Mesoporous Sulfonic Acid Functionalized ZrO2/organosilica Bifunctional Catalysts for Direct Catalytic Conversion of Glucose to Ethyl Levulinate

Isobutane Dehydrogenation Assisted by CO2 over Silicalite‐1‐Supported ZnO Catalysts: Influence of Support Crystallite Size

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Design of Ordered Mesoporous Sulfonic Acid Functionalized ZrO₂/organosilica Bifunctional Catalysts for Direct Catalytic Conversion of Glucose to Ethyl Levulinate

Isobutane Dehydrogenation Assisted by CO₂ over Silicalite‐1‐Supported ZnO Catalysts: Influence of Support Crystallite Size