Catalysis on Zeolites and Zeolite-Like Materials

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Catalytic Materials".

Deadline for manuscript submissions: closed (10 May 2022) | Viewed by 30137

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Guest Editor
Fakultät Chemie und Lebensmittelchemie, Technische Universität Dresden, Helmholtzstraße 14, 01069 Dresden, Germany
Interests: heterogeneous catalysis; zeolites; micro/mesoporous aluminosilicates; microreactor systems; flow chemistry; green chemistry
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Special Issue Information

Dear Colleagues,

The journal Catalysts plans to publish a Special Issue entitled “Catalysis on Zeolites and Zeolite-Like Materials”. The first use of zeolite catalysts occurred 60 years ago when researchers of Union Carbide Corp. tested zeolite Y as an isomerization catalyst. The followed introduction of zeolite-based catalysts in fluid catalytic cracking processes remains the largest application of zeolites in catalysis. Over the past decades progress in zeolite synthesis enabled the discovery of new zeolite types, which allowed for the development of new catalytic processes in petrochemical industries. Moreover, new tools for zeolite modification allowed for additional applications of zeolite-based catalysts in the field of environmental catalysis. The development of new mesoporous and micro/mesoporous or zeolite-like materials, such as metal–organic frameworks, as well as progress in computational chemistry and solid state characterization techniques demonstrated that the potential of ordered pore materials is still far from exhausted, and that further biocatalysis, electrocatalysis, photocatalysis, and micro/nanostructure technology indicate increasing interest in this class of substances.

With great pleasure, I invite you to submit your manuscript to the Special Issue “Catalysis on Zeolites and Zeolite-Like Materials”, to share developments and recent progress regarding the synthesis, characterization and application of zeolites or zeolite-like materials as catalysts.

Prof. Dr. Wladimir Reschetilowski
Guest Editor

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Keywords

  • zeolites and zeolite-like materials
  • acid–base catalysis
  • bifunctional catalysis
  • environmental catalysis
  • biocatalysis
  • electrocatalysis
  • photocatalysis
  • C1 chemistry
  • kinetic modeling of zeolite-catalyzed chemical reactions
  • computation in catalysis with ordered porous materials

Published Papers (11 papers)

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Editorial

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4 pages, 168 KiB  
Editorial
Catalysis on Zeolites and Zeolite-like Materials
by Wladimir Reschetilowski
Catalysts 2024, 14(2), 128; https://doi.org/10.3390/catal14020128 - 7 Feb 2024
Viewed by 1132
Abstract
When the Swedish mineralogist Axel F [...] Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)

Research

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11 pages, 11722 KiB  
Article
Protolytic Ring-Opening Cracking of Methylcyclohexane over Hierarchical High-Silica USY Zeolite: A Haag-Dessau Cracking
by Yaojie Li, Bo Qin, Wenming Hao, Yanze Du, Jinghong Ma and Ruifeng Li
Catalysts 2022, 12(7), 697; https://doi.org/10.3390/catal12070697 - 25 Jun 2022
Cited by 2 | Viewed by 1430
Abstract
To reveal the influence of acid sites with different spatial locations of USY zeolite with different micro-/mesoporous structures and Si/Al ratio, catalytic cracking of methylcyclohexane on the zeolites is employed to study the synergism effects of acid sites and porous structures (“active region”) [...] Read more.
To reveal the influence of acid sites with different spatial locations of USY zeolite with different micro-/mesoporous structures and Si/Al ratio, catalytic cracking of methylcyclohexane on the zeolites is employed to study the synergism effects of acid sites and porous structures (“active region”) in the hierarchical USY zeolites. The results showed that the hierarchical USY zeolites have increased numbers of accessibly strong Brønsted acid sites and greatly enhanced diffusion ability due to the hierarchical pore-structure, resulting in mainly monomolecular protolytic scission in cracking reactions and less bimolecular hydrogen transfer. The isomerization reaction is from intramolecular transalkylation and the isomerics are the intermediates of the cracking reaction. The protolytic cracking that occurs in hierarchical high-silica USY-zeolites follows the Haag-Dessau cracking. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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13 pages, 2727 KiB  
Article
Critical Role of Al Pair Sites in Methane Oxidation to Methanol on Cu-Exchanged Mordenite Zeolites
by Peijie Han, Zhaoxia Zhang, Zheng Chen, Jingdong Lin, Shaolong Wan, Yong Wang and Shuai Wang
Catalysts 2021, 11(6), 751; https://doi.org/10.3390/catal11060751 - 19 Jun 2021
Cited by 5 | Viewed by 3037
Abstract
Cu-exchanged aluminosilicate zeolites have been intensively studied for the selective oxidation of methane to methanol via a chemical looping manner, while the nature of active Cu-oxo species for these catalysts is still under debate. This study inquired into the effects of Al distribution [...] Read more.
Cu-exchanged aluminosilicate zeolites have been intensively studied for the selective oxidation of methane to methanol via a chemical looping manner, while the nature of active Cu-oxo species for these catalysts is still under debate. This study inquired into the effects of Al distribution on methane oxidation over Cu-exchanged aluminosilicate zeolites, which provided an effective way to discern the activity difference between mononuclear and polynuclear Cu-oxo species. Specifically, conventional Na+/Co2+ ion-exchange methods were applied to quantify isolated Al and Al pair (i.e., Al−OH−(Si−O)1–3−Al−OH) sites for three mordenite (MOR) zeolites, and a correlation was established between the reactivity of the resultant Cu-MOR catalysts and the portions of the accessible framework Al sites. These results indicated that the Cu-oxo clusters derived from the Al pair sites were more reactive than the CuOH species grafted at the isolated Al sites, which is consistent with in situ ultraviolet-visible spectroscopic characterization and density functional theory calculations. Further theoretical analysis of the first C–H bond cleavage in methane on these Cu-oxo species unveiled that stabilization of the formed methyl group was the predominant factor in determining the reactivity of methane oxidation. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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18 pages, 3156 KiB  
Article
Kinetics of n-Hexane Cracking over Mesoporous HY Zeolites Based on Catalyst Descriptors
by Yann Chapellière, Cécile Daniel, Alain Tuel, David Farrusseng and Yves Schuurman
Catalysts 2021, 11(6), 652; https://doi.org/10.3390/catal11060652 - 21 May 2021
Cited by 10 | Viewed by 2451
Abstract
A simple kinetic model based on the zeolite acid strength, the number of Brønsted acid sites, and the catalyst efficiency was developed for the cracking of n-hexane. A series of HY zeolites with a mesopore volume from 0.04 to 0.32 cm3 [...] Read more.
A simple kinetic model based on the zeolite acid strength, the number of Brønsted acid sites, and the catalyst efficiency was developed for the cracking of n-hexane. A series of HY zeolites with a mesopore volume from 0.04 to 0.32 cm3/g was synthesized and characterized by various physical-chemical methods and tested for n-hexane cracking. The generation of mesoporosity influenced several other important parameters, such as acidity and extra-framework aluminum. Zero-length column diffusion measurements for mesitylene showed a large decrease in the characteristic diffusion time upon the introduction of mesoporosity, which changed only slightly with a further increase in mesoporosity. Similar n-hexane physisorption enthalpies were measured for all samples. The highest initial activity for n-hexane cracking per catalyst volume was observed for the sample with an intermediate mesopore volume of 0.15 cm3/g. The three mesoporous H-USY zeolites showed the same value of the intrinsic rate constant and the same activation energy. The difference in initial activity of the mesoporous zeolites was caused by the difference in the number of Brønsted acid sites. The increase in initial activity for the mesoporous zeolites compared to a microporous zeolite was caused by an increase in the acid strength. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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13 pages, 3801 KiB  
Article
Ionothermal Synthesis of Triclinic SAPO-34 Zeolites
by Li Han, Xinxin Yan, Lulu Guo, Yanan Duan, Zheng Wang, Tianliang Lu, Jun Xu, Yuzhong Zhan and Jianfeng Wang
Catalysts 2021, 11(5), 616; https://doi.org/10.3390/catal11050616 - 11 May 2021
Cited by 9 | Viewed by 2470
Abstract
A triclinic SAPO-34 molecular sieve was synthesized ionothermally. The as-synthesized products were characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), nuclear magnetic resonance (NMR), fourier infrared spectrometer (FT-IR) and thermogravimetric (TG) analyses. The formation mechanism of the hierarchical porous triclinic SAPO-34 [...] Read more.
A triclinic SAPO-34 molecular sieve was synthesized ionothermally. The as-synthesized products were characterized by powder X-ray diffraction (XRD), scanning electron microscope (SEM), nuclear magnetic resonance (NMR), fourier infrared spectrometer (FT-IR) and thermogravimetric (TG) analyses. The formation mechanism of the hierarchical porous triclinic SAPO-34 zeolites and the factors affecting the morphology of the SAPO-34 molecular sieve were investigated. The results show that the formation mechanism of the hierarchical pores is in accordance with Ostwald ripening theory, and the accumulation of grains constitutes the existence of mesopores and macropores. The crystallization temperature, ionic liquid type, and organic amines can effectively change the morphology and crystallinity of the SAPO-34 molecular sieve. The crystallization temperature, ionic liquid and template have great influence on the (111) crystal plane, thus affecting the morphology of the molecular sieve. Moreover, it can be proven through NMR and TG analyses that ionic liquids and organic amines can be used as structure directing agents together. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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19 pages, 2885 KiB  
Article
Layer-Like Zeolite X as Catalyst in a Knoevenagel Condensation: The Effect of Different Preparation Pathways and Cation Exchange
by Jan-Paul Grass, Katharina Klühspies, Bastian Reiprich, Wilhelm Schwieger and Alexandra Inayat
Catalysts 2021, 11(4), 474; https://doi.org/10.3390/catal11040474 - 7 Apr 2021
Cited by 6 | Viewed by 2403
Abstract
This study is dedicated to the comparative investigation of the catalytic activity of layer-like Faujasite-type (FAU) zeolite X obtained from three different synthesis routes (additive-free route, Li2CO3 route, and TPOAC route) in a liquid-phase Knoevenagel condensation of benzaldehyde and ethyl [...] Read more.
This study is dedicated to the comparative investigation of the catalytic activity of layer-like Faujasite-type (FAU) zeolite X obtained from three different synthesis routes (additive-free route, Li2CO3 route, and TPOAC route) in a liquid-phase Knoevenagel condensation of benzaldehyde and ethyl cyanoacetate to ethyl trans-α-cyanocinnamate. It is shown that the charge-balancing cations (Na+ and K+) and the morphological properties have a strong influence on the apparent reaction rate and degree of conversion. The highest initial reaction rate could be found for the layer-like zeolite X synthesised by the additive-free route in the potassium form. In most cases, the potassium-exchanged zeolites enabled higher maximum conversions and higher reaction rates compared to the zeolite X catalysts in sodium form. However, very thin crystal plates (below 100 nm thickness), similar to those obtained in the presence of TPOAC, did not withstand the multiple aqueous ion exchange procedure, with the remaining coarse crystals facilitating less enhancement of the catalytic activity. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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20 pages, 3880 KiB  
Article
Conversion of Oxygenates on H-ZSM-5 Zeolites—Effects of Feed Structure and Si/Al Ratio on the Product Quality
by Torsten Gille, Markus Seifert, Mathias S. Marschall, Sascha Bredow, Tobias Schneider, Oliver Busse, Wladimir Reschetilowski and Jan J. Weigand
Catalysts 2021, 11(4), 432; https://doi.org/10.3390/catal11040432 - 28 Mar 2021
Cited by 6 | Viewed by 2811
Abstract
The conversion of different biogenic feedstocks to hydrocarbons is a major challenge when ensuring hydrocarbon and fuel supply in spite of the heterogeneity of this feed. Flexible adaptation to changing compositions is mandatory for the respective processes. In this study, different oxygenate model [...] Read more.
The conversion of different biogenic feedstocks to hydrocarbons is a major challenge when ensuring hydrocarbon and fuel supply in spite of the heterogeneity of this feed. Flexible adaptation to changing compositions is mandatory for the respective processes. In this study, different oxygenate model feeds, such as alcohols, aldehydes, carboxylic acids and esters, were converted at 500 °C and 5 barg H2 using H-ZSM-5 zeolite catalysts with various Si/Al ratios to identify the relationship between the feed structure and the final product distribution. As the main outcome, the product distribution becomes increasingly independent of the feed structure for Al-rich H-ZSM-5 catalyst samples at low Time on Stream (ToS). Some minor exceptions are the increased formation of aromatics during ToS for carbonyl oxygenates compared to primary alcohols and the dominance of initial deoxygenation products for Si-rich H-ZSM-5 samples. This is interpreted by a multi-stage reaction sequence, which involves the initial deoxygenation of the feed and the subsequent integration of the olefin intermediates into a reaction network. The results pave the way towards the achievement of a desired product distribution in the conversion of different oxygenates simply by the adaption of the Al content of H-ZSM-5. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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22 pages, 2687 KiB  
Article
Promotional Effect of Pd Addition on the Catalytic Activity of Composite Pt-Pd/AlSBA-15–β Catalyst for Enhanced n-Heptane Hydroisomerization
by Karolina Jaroszewska, Monika Fedyna, Aleksandra Masalska, Rafał Łużny and Janusz Trawczyński
Catalysts 2021, 11(3), 377; https://doi.org/10.3390/catal11030377 - 13 Mar 2021
Cited by 5 | Viewed by 2750
Abstract
Hierarchical AlSBA-15–zeolite materials were utilized as a supports for preparing hydroisomerization catalysts. Detailed consideration was given to: (i) the effect of the zeolite type introduced into AlSBA-15–zeolite composites (where zeolite is β, mordenite or ZSM-5) as well as (ii) the promotion effect of [...] Read more.
Hierarchical AlSBA-15–zeolite materials were utilized as a supports for preparing hydroisomerization catalysts. Detailed consideration was given to: (i) the effect of the zeolite type introduced into AlSBA-15–zeolite composites (where zeolite is β, mordenite or ZSM-5) as well as (ii) the promotion effect of Pd addition. The composites showed higher activity in isomerization as compared to Pt/AlSBA-15. The enhanced isomerization efficiency were explained by the appropriate metallic and acidic function as well as suitable transport properties. The modification of the hydrogenating function by Pd incorporation increases the hydroisomerization efficiency of Pt-Pd/AlSBA-15–β catalyst. Over bimetallic Pt-Pd/AlSBA-15–β, the high yields of isomers (68 wt%) with respect to 50 wt% for a control catalyst. The most promising Pt-Pd/AlSBA-15–β catalyst allows to improve research octane number from 0 to the 74 value. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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15 pages, 3249 KiB  
Article
Influence of Remaining Acid Sites of an Amorphous Aluminosilicate on the Oligomerization of n-Butenes after Impregnation with Nickel Ions
by Fabian Nadolny, Felix Alscher, Stephan Peitz, Ekaterina Borovinskaya, Robert Franke and Wladimir Reschetilowski
Catalysts 2020, 10(12), 1487; https://doi.org/10.3390/catal10121487 - 21 Dec 2020
Cited by 4 | Viewed by 2630
Abstract
Highly linear octene isomers can be produced from n-butene on industrial scale by using Ni-containing aluminosilicates as heterogeneous catalysts. These catalysts can be prepared by impregnating an aluminosilicate with a Ni(II) salt solution. This leads to a competition between acid-catalyzed and nickel-catalyzed reactions. [...] Read more.
Highly linear octene isomers can be produced from n-butene on industrial scale by using Ni-containing aluminosilicates as heterogeneous catalysts. These catalysts can be prepared by impregnating an aluminosilicate with a Ni(II) salt solution. This leads to a competition between acid-catalyzed and nickel-catalyzed reactions. In this study it is shown that some octene isomers are exclusively formed via an acid-catalyzed mechanism as a result of methyl group migration at the surface of a mesoporous catalyst. Specifically, the isomers 4,4-dimethylhexene (4,4-DMH) and 3-ethyl-2-methylpentene (3E-2MP) exhibit a systematic correlation compared to the amount of 3,4-dimethylhexene (3,4-DMH) formed at acid sites. By analyzing the ratio of 4,4-DMH and/or 3E-2MP to 3,4-DMH in the product spectrum before and after impregnation with a nickel precursor, the extend of acid site covered by nickel ions can be evaluated. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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16 pages, 1937 KiB  
Article
Catalytic Formation of Lactic and Levulinic Acids from Biomass Derived Monosaccarides through Sn-Beta Formed by Impregnation
by Andrew Kohler, Wayne Seames, Ian Foerster and Clancy Kadrmas
Catalysts 2020, 10(10), 1219; https://doi.org/10.3390/catal10101219 - 20 Oct 2020
Cited by 9 | Viewed by 2865
Abstract
In the present study, the use of Sn-Beta zeolite to facilitate the conversion of lignocellulosic biomass-derived glucose and xylose into lactic and levulinic acid was explored. The reactions were carried out in a batch reactor using water as the solvent. Water is the [...] Read more.
In the present study, the use of Sn-Beta zeolite to facilitate the conversion of lignocellulosic biomass-derived glucose and xylose into lactic and levulinic acid was explored. The reactions were carried out in a batch reactor using water as the solvent. Water is the preferred solvent over methanol as it reduces downstream product acid recovery and purification complexity. Optimization experiments were performed for reaction temperature and residence time. Under optimized reaction conditions, the Sn-Beta facilitated reaction of a pure sugar solution resulted in lactic acid yields of 13 and 19 wt% of inlet carbon of glucose and xylose, respectively, plus levulinic acid yields of 18 and 0.8 wt%, respectively. When actual biomass-derived sugar solutions were tested, the yields of lactic acid were significantly higher than those from the optimized model solution experiments with lactic acid yields of 34 wt%. These biomass-derived sugar solutions contained residual levels of CaSO4 from the neutralization step of the hydrolysis process. Further experiments were performed to examine the potential effects from CaSO4 contributing to this increase. It was found that the sulfate ions increased the Brønsted basicity and the calcium increased the Lewis acidity of the reaction solution, and that the combination of both effects increased the conversion of the original sugars into lactic acid. These effects were verified by testing other organic bases to isolate the Brønsted acid neutralization effect and the Lewis acid enhancement effect. The addition of CaSO4 resulted in attractive lactic acid yields, 68 wt% and 50 wt% of inlet carbon from pure glucose and xylose solutions, respectively. Increasing the actual corn stover and forage sorghum derived sugars concentration (in water) allowed lactic acids yields of greater than 60 wt% to be achieved. When the optimized Sn-Beta reaction system was applied to corn stover and forage sorghum mixtures, it was found that the ratio of lactic-to-levulinic acid generated was inversely dependent upon the glucose-to-xylose ratio in the recovered sugar mixture. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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12 pages, 2255 KiB  
Article
Hydrocracking of Light Diesel Oil over Catalysts with Industrially Modified Y Zeolites
by Mengna Zhang, Bo Qin, Weimin Zhang, Jiajun Zheng, Jinghong Ma, Yanze Du and Ruifeng Li
Catalysts 2020, 10(8), 815; https://doi.org/10.3390/catal10080815 - 22 Jul 2020
Cited by 8 | Viewed by 3981
Abstract
Three industrially modified Y zeolites with a hierarchical structure were characterized by XRD, N2 adsorption–desorption, SEM, TEM, 27Al-/29Si-NMR, in situ pyridine-FTIR, and NH3-TPD techniques. The industrial hydrocracking catalyst of light diesel oil was prepared by kneading and [...] Read more.
Three industrially modified Y zeolites with a hierarchical structure were characterized by XRD, N2 adsorption–desorption, SEM, TEM, 27Al-/29Si-NMR, in situ pyridine-FTIR, and NH3-TPD techniques. The industrial hydrocracking catalyst of light diesel oil was prepared by kneading and extruding the mixture of 10 wt.% industrially modified zeolite, commercial alumina, nickel nitrate, and molybdenum oxide. The small amount of hierarchical Y zeolite in the hydrocracking catalyst plays a key role, resulting in selective hydrogenation of naphthalene and further ring-opening activity. The mesoporous structure of the zeolites provided an effective interface and improved the accessibility of acid sites to bulky reactants. Full article
(This article belongs to the Special Issue Catalysis on Zeolites and Zeolite-Like Materials)
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