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Catalysts
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Microporous and Mesoporous Materials for Catalytic Applications
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Microporous and Mesoporous Materials for Catalytic Applications

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

Deadline for manuscript submissions: 30 June 2024 | Viewed by 17460

Special Issue Editor

Dr. Narendra Kumar

E-Mail Website
Guest Editor
Faculty of Science and Engineering, Industrial Chemistry and Reaction Engineering, Åbo Akademi University, Henriksgatan 2, FI-20500 Turku, Finland
Interests: heterogeneous catalysis; catalyst synthesis; nanoporous materials; catalyst characterization; zeolite catalysis; refinery processes; hydrocarbon conversion; reaction mechanism; biomass transformations
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Microporous and mesoporous materials, due to their unique properties (uniform pores, channel systems, shape selectivity and high thermal stability), have found applications as catalytic materials in several oil refinery processes, in the production of petrochemicals, fine chemicals, pharmaceuticals, drug molecules and specialty chemicals. Furthermore, possibilities to design catalytic active metal sites with well-defined size, dispersion and location in microporous and mesoporous materials have attracted the interest of researchers in academia and industry. The Brønsted and Lewis acid sites in microporous and mesoporous materials can be varied by changing the silica to alumina ratio, which gives the possibilities to tailor the acid sites with given amounts and strengths. Metal-modified and acidic microporous and mesoporous materials after deactivation in reaction are easily regenerated and reused, thus making them highly efficient and cost-effective catalytic materials.

Dr. Narendra Kumar
Guest Editor

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Keywords

  • microporous materials
  • mesoporous materials
  • catalysts
  • synthesis
  • catalysis
  • characterization
  • chemicals
  • fuels

Published Papers (9 papers)

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Research

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23 pages, 7487 KiB  
Article
Hydrodesulfurization of Thiophene in n-Heptane Stream Using CoMo/SBA-15 and CoMo/AlSBA-15 Mesoporous Catalysts
by Ana Carla S. L. S. Coutinho, Joana M. F. Barros, Marcio D. S. Araujo, Jilliano B. Silva, Marcelo J. B. Souza, Regina C. O. B. Delgado, Valter J. Fernandes Jr. and Antonio S. Araujo
Catalysts 2024, 14(3), 198; https://doi.org/10.3390/catal14030198 - 18 Mar 2024
Viewed by 1197
Abstract
Heterogeneous catalysts containing cobalt and molybdenum supported on mesoporous materials types SBA-15 and AlSBA-15 were synthesized for application in the HDS reactions of thiophene in the n-heptane stream. The materials were synthesized by the hydrothermal method using Pluronic P123 as a template. The [...] Read more.
Heterogeneous catalysts containing cobalt and molybdenum supported on mesoporous materials types SBA-15 and AlSBA-15 were synthesized for application in the HDS reactions of thiophene in the n-heptane stream. The materials were synthesized by the hydrothermal method using Pluronic P123 as a template. The calcined SBA-15 and AlSBA-15 supports were submitted to co-impregnation with solutions of cobalt nitrate and ammonium heptamolybdate, aiming for the production of 15% in mass of metal loading with an atomic ratio of [Co/(Co + Mo)] = 0.45. The obtained materials were dried and calcined to obtain the mesoporous catalysts in the forms of CoMo/SBA-15 and CoMo/AlSBA-15. The catalysts were characterized by XRD, TG/DTG, SEM, and nitrogen adsorption. From XRD analysis, it was verified that after the decomposition of the cobalt and molybdenum salts, MoO3, Co3O4, and CoMoO4 oxides were formed on the supports, being attributed to these chemical species, the activity for the HDS reactions. The catalytic activity of the obtained catalysts was evaluated in a continuously flowing tubular fixed-bed microreactor coupled on-line to a gas chromatograph, using an n-heptane stream containing 12,070 ppm of thiophene (ca. 5100 ppm of sulfur) as a model compound. The synthesized catalysts presented suitable activity for the HDS reaction, and the main obtained products were cis- and trans-2-butene, 1-butene, n-butane, and low amounts of isobutane. The presence of 1,3-butadiene and tetrahydrothiophene (THT) was not detected. A mechanism of the primary and secondary reactions and subsequent formation of the olefins and paraffins in the CoMo/SBA-15 and CoMo/AlSBA-15 mesoporous catalysts was proposed, considering steps of desulfurization, hydrogenation, dehydrogenation, THT decyclization, and isomerization. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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17 pages, 1944 KiB  
Article
Dimethyl Ether to Olefins on Hybrid Intergrowth Structure Zeolites
by Maria V. Magomedova, Anastasiya V. Starozhitskaya, Ilya A. Davidov, Dmitry E. Tsaplin and Anton L. Maximov
Catalysts 2023, 13(3), 570; https://doi.org/10.3390/catal13030570 - 11 Mar 2023
Cited by 1 | Viewed by 1187
Abstract
A series of catalysts based on hybrid intergrowth structure zeolites MFI-MEL, MFI-MTW, and MFI-MCM-41 are studied in the reaction of olefins synthesis from dimethyl ether at atmospheric pressure and a temperature of 340 °C. The total acidity of hybrid zeolite-based catalysts is shown [...] Read more.
A series of catalysts based on hybrid intergrowth structure zeolites MFI-MEL, MFI-MTW, and MFI-MCM-41 are studied in the reaction of olefins synthesis from dimethyl ether at atmospheric pressure and a temperature of 340 °C. The total acidity of hybrid zeolite-based catalysts is shown to correlate with their activity. However, the use of zeolite with the structure MFI-MCM-41, which is characterized by a high content of medium acid sites, additionally catalyzes the methanol dehydration reaction, resulting in a decrease in the observed DME conversion. The obtained product distributions are brought into correlation with the texture of catalysts. It is shown that the use of hybrid zeolites does not change the mechanism of reaction, but the structural features of zeolites influence the priority of the competing MTO reactions: high ethylene yield is observed for catalysts with high micropore volume. The topology of the hybrid zeolite has been shown to influence the hydrogen transfer reaction rate, but not to change the isomerizing activity of the catalyst. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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18 pages, 4164 KiB  
Article
Catalytic Distillation of Atmospheric Residue of Petroleum over HY-MCM-41 Micro-Mesoporous Materials
by Camila G. D. P. Morais, Jilliano B. Silva, Josue S. Almeida, Rafaela R. Oliveira, Marcio D. S. Araujo, Glauber J. T. Fernandes, Regina C. O. B. Delgado, Ana C. F. Coriolano, Valter J. Fernandes, Jr. and Antonio S. Araujo
Catalysts 2023, 13(2), 296; https://doi.org/10.3390/catal13020296 - 28 Jan 2023
Cited by 2 | Viewed by 2268
Abstract
Catalytic distillation is a technology that combines a heterogeneous catalytic reaction and the separation of reactants and products via distillation in a single reactor/distillation system. This process combines catalysis, kinetics, and mass transfer to obtain more selective products. The heterogeneous catalyst provides the [...] Read more.
Catalytic distillation is a technology that combines a heterogeneous catalytic reaction and the separation of reactants and products via distillation in a single reactor/distillation system. This process combines catalysis, kinetics, and mass transfer to obtain more selective products. The heterogeneous catalyst provides the sites for catalytic reactions and the porous surface for liquid/vapor separation. The advantages of catalytic distillation are energy savings, low waste streams, catalyst longevity, higher conversion, and product selectivity; these properties are interesting for petrochemical and petroleum industries. For this study, 100 mL of atmospheric residue of petroleum (ATR) was distilled in the presence of 1.0 g of a micro/mesoporous catalyst composed of a HY-MCM-41, and the reactor used was an OptiDist automatic distillation device, operating according to ASTM D-86 methodology. The products were collected and analyzed by gas chromatography. The samples of ATR, HY/ATR, and HY-MCM-41/ATR were analyzed by thermogravimetry (TG) to determine the activation energies (Ea) relative to the thermal decomposition of the process, using the Ozawa–Flynn–Wall (OFW) kinetic model. The obtained results show a potential catalytic distillation system for use in the reaction of heavy petroleum fractions and product separation from the HY/MCM-41 micro/mesoporous catalyst. The TG data revealed two mass loss events for ATR in the ranges of 100–390 and 390–590 °C, corresponding to volatilization and thermal cracking, respectively. The Ea determined for the thermal degradation of the ATR without a catalyst was in the range of 83–194 kJ/mol, whereas in the presence of the HY-MCM-41 catalyst, it decreased to 61–105 kJ/mol, evidencing the catalytic effect of the micro-mesoporous material. The chromatography analysis allowed for the identification of gasoline and a major production of diesel and gasoil when the HY-MCM-41 mixture was used as the catalyst, evidencing the synergism of the combined effect of the acid sites, the crystalline phase, and the microporosity of the HY zeolite with the accessibility of the hexagonal mesoporous structure of the MCM-41 material. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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23 pages, 10242 KiB  
Article
Effect of Basic Promoters on Porous Supported Alumina Catalysts for Acetins Production
by Rita de Cássia F. Bezerra, Gabriela Mota, Ruth Maria B. Vidal, Jose Vitor do Carmo, Gilberto D. Saraiva, Adriana Campos, Alcineia C. Oliveira, Rossano Lang, Larissa Otubo, José Jiménez Jiménez and Enrique Rodríguez-Castellón
Catalysts 2022, 12(12), 1616; https://doi.org/10.3390/catal12121616 - 09 Dec 2022
Cited by 2 | Viewed by 1337
Abstract
A facile strategy for the design of porous supports was obtained by modifying the sol-gel method followed by the wet impregnation technique. In this respect, herein, the acidity of the γ-Al2O3 phase was modulated by adding basic MgO, La2 [...] Read more.
A facile strategy for the design of porous supports was obtained by modifying the sol-gel method followed by the wet impregnation technique. In this respect, herein, the acidity of the γ-Al2O3 phase was modulated by adding basic MgO, La2O3 or ZnO promoters to form binary supported catalysts. The Ni and Co dispersion on the supports associated with their tunable acidity and morphologies resulted in highly porous supported alumina-based catalysts. The physicochemical properties of the solids were comprehensively investigated by XRD, textural properties, Raman and FTIR spectroscopy, SEM-EDS, TEM, EPR and XPS analyses. The catalytic performances in the esterification of glycerol in the presence of acetic acid (EG) for the acetins production were evaluated. The highly dispersed NiO and Co3O4 active species on binary porous supports produced synergistic effects appearing to be the reason for the activity of the solids in the EG reaction. Under the optimized reaction conditions, NiCo/MgO-Al2O3 was found to be a robust solid with superior catalytic performance and improved stability in four reaction cycles with 65.0% of glycerol conversion with an exclusive selectivity of 53% for triacetin. The presence of Co2+/Co3+ and Ni2+ strongly interacting with the spinel γ-Al2O3 and MgAl2O4 phases, the latter having a large number of lattice oxygen species, was considered another active component besides those of Ni and Co in the esterification of glycerol. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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13 pages, 2944 KiB  
Article
Ni and Ce Grafted Ordered Mesoporous Silica KIT-6 for CO2 Adsorption
by Mariana Suba, Alexandru Popa, Orsina Verdeș, Silvana Borcănescu and Paul Barvinschi
Catalysts 2022, 12(11), 1339; https://doi.org/10.3390/catal12111339 - 01 Nov 2022
Cited by 3 | Viewed by 1502
Abstract
In this study, the Ni/KIT-6 and Ce/KIT-6 materials were prepared through the impregnation method and then amino-functionalized materials were obtained by the grafting of an amino-silane coupling agent 3-aminopropyl triethoxysilane (APTES). The samples were characterized by thermogravimetric analysis (TGA-DTA), Fourier transform infrared spectroscopy [...] Read more.
In this study, the Ni/KIT-6 and Ce/KIT-6 materials were prepared through the impregnation method and then amino-functionalized materials were obtained by the grafting of an amino-silane coupling agent 3-aminopropyl triethoxysilane (APTES). The samples were characterized by thermogravimetric analysis (TGA-DTA), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction, scanning electron microscopy (SEM) and nitrogen adsorption at 77 K. The study of CO2 adsorption–desorption on prepared materials was investigated using thermogravimetric analysis (TGA-DTA) coupled with mass spectrometry (MS). The influence of metal oxides on the performance of CO2 adsorption on functionalized mesoporous silica was presented. The results showed that doping the molecular sieve with cerium oxide can significantly increase the adsorption capacity of the amino-functionalized KIT-6. As the CO2 adsorbents were prepared by functionalization through grafting with APTES, the amount of amine loading is one of the important factors which improves CO2 adsorption capacity. Additionally, CO2 adsorption performance depends on the textural properties and the temperature used for the adsorption process. The maximum adsorption capacity of Ce/KIT-6 Sil is 3.66 mmol/g, which is 2.4 times higher than Ni/KIT-6 Sil. After the nine cycles of cyclic CO2 adsorption/desorption, the Ce/KIT-6 Sil still had higher adsorption capacities, indicating their good cyclical stability. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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22 pages, 5210 KiB  
Article
Ordered Mesoporous nZVI/Zr-Ce-SBA-15 Catalysts Used for Nitrate Reduction: Synthesis, Optimization and Mechanism
by Ruimin Zhang, Haixia Liu, Weili Jiang and Weijing Liu
Catalysts 2022, 12(7), 797; https://doi.org/10.3390/catal12070797 - 19 Jul 2022
Cited by 2 | Viewed by 1404
Abstract
Excessive concentrations of nitrate (NO3-N) in water lead to the deterioration of water quality, reducing biodiversity and destroying ecosystems. Therefore, the present study investigated NO3-N removal from simulated wastewater by nanoscale zero-valent iron-supported ordered mesoporous Zr-Ce-SBA-15 composites (nZVI/Zr-Ce-SBA-15) assisted [...] Read more.
Excessive concentrations of nitrate (NO3-N) in water lead to the deterioration of water quality, reducing biodiversity and destroying ecosystems. Therefore, the present study investigated NO3-N removal from simulated wastewater by nanoscale zero-valent iron-supported ordered mesoporous Zr-Ce-SBA-15 composites (nZVI/Zr-Ce-SBA-15) assisted by response surface methodology (RSM), an artificial neural network combined with a genetic algorithm (ANN-GA) and a radial basis neural network (RBF). The successful support of nZVI on Zr-Ce-SBA-15 was confirmed using XRD, FTIR, TEM, SEM–EDS, N2 adsorption and XPS, which indicated ordered mesoporous materials. The results showed that ANN-GA was better than the RSM for optimizing the conditions of NO3-N removal and the RBF neural network further confirmed the reliability of the ANN-GA model. The removal rate of NO3-N by the composites reached 95.71% under the optimized experimental conditions (initial pH of 4.89, contact time = of 62.27 min, initial NO3-N concentration of 74.84 mg/L and temperature of 24.77 °C). The process of NO3-N adsorption onto Zr-Ce-SBA-15 composites was followed by the Langmuir model (maximum adsorption capacity of 45.24 mg/g), pseudo-second-order kinetics, and was spontaneous, endothermic and entropy driven. The yield of N2 can be improved after nZVI was supported on Zr-Ce-SBA-15, and the composites exhibited a strong renewability in the short term within three cycles. The resolution of Fe2+ experiments confirmed that nZVI/Zr-Ce-SBA-15 was simultaneously undergoing adsorption and catalysis in the process of NO3-N removal. Our study suggests that the ordered mesoporous nZVI/Zr-Ce-SBA-15 composites are a promising material for simultaneously performing NO3-N removal and improving the selectivity of N2, which provides a theoretical reference for NO3-N remediation from wastewater. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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Review

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39 pages, 10612 KiB  
Review
Porous Aerogel Structures as Promising Materials for Photocatalysis, Thermal Insulation Textiles, and Technical Applications: A Review
by Kang Hoon Lee, Zafar Arshad, Alla Dahshan, Mubark Alshareef, Qana A. Alsulami, Ayesha Bibi, Eui-Jong Lee, Muddasir Nawaz, Usman Zubair and Amjed Javid
Catalysts 2023, 13(9), 1286; https://doi.org/10.3390/catal13091286 - 08 Sep 2023
Cited by 5 | Viewed by 2250 | Correction
Abstract
Aerogels, due to their unique features like lightweight, ultra-low thermal conductivity, and design variations, have gotten a lot of interest in thermal insulation, photocatalysis, and protective areas. Besides their superior thermal properties, aerogel thermal insulation and photocatalyst materials also possess many inherent flaws, [...] Read more.
Aerogels, due to their unique features like lightweight, ultra-low thermal conductivity, and design variations, have gotten a lot of interest in thermal insulation, photocatalysis, and protective areas. Besides their superior thermal properties, aerogel thermal insulation and photocatalyst materials also possess many inherent flaws, such as handling issues, high manufacturing costs, and low strength as well as toughness. The most persuasive and successful ways to improve photocatalytic and thermal insulating qualities while lowering costs are composition optimization and microstructure reconstruction. Their high surface area and porosity make them ideal for enhancing the efficiency and capacity of these devices. Research may lead to more efficient and longer-lasting energy storage solutions. This review describes the characteristics, microstructural reconstruction, design variation, and properties of all aerogel fabrication techniques and provides a comprehensive overview of scientific achievements linked to them. The effectiveness of raw material compositions, properties, and mechanical parameters are also discussed. The major goal of this review is to highlight the aerogel-based materials and design variations and to explore the most potential development trends for photocatalysis and thermal applications. The industrial as well as technical applications of silica aerogels are also highlighted. This review highlights futuristic applications of aerogel-based textile materials to alleviate the CO2 burden on our atmosphere, either by providing next-level thermal insulation or by employing them in CO2 mitigating technologies such as CO2 capture. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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28 pages, 4647 KiB  
Review
Hierarchical Zeolite Synthesis by Alkaline Treatment: Advantages and Applications
by Daniele S. Oliveira, Rafael B. Lima, Sibele B. C. Pergher and Vinícius P. S. Caldeira
Catalysts 2023, 13(2), 316; https://doi.org/10.3390/catal13020316 - 01 Feb 2023
Cited by 8 | Viewed by 2922
Abstract
Zeolites are of great interest to the scientific and industrial communities due to their interesting catalytic properties, such as high specific area, shape selectivity, and thermal and hydrothermal stability. For this reason, zeolites have been intensively studied and applied in several reactions of [...] Read more.
Zeolites are of great interest to the scientific and industrial communities due to their interesting catalytic properties, such as high specific area, shape selectivity, and thermal and hydrothermal stability. For this reason, zeolites have been intensively studied and applied in several reactions of great industrial interest. However, the size of zeolite micropores may hinder the diffusion of bulky molecules in the pore system, limiting the use of zeolites in some reactions/applications that use bulky molecules. One way to address this limitation is to generate secondary porosity (in the range of supermicropores, mesopores and/or macropores) in such a way that it connects with the existing micropores, creating a hierarchical pore system. There are different hierarchical approaches; however, most are not economically viable and are complicated/time-consuming. Alkaline treatment has been highlighted in recent years due to its excellent results, simplicity, speed and low cost. In this review, we highlight the importance of alkaline treatment in the generation of secondary porosity and the parameters that influence alkaline treatment in different zeolitic structures. The properties and catalytic performance of hierarchical zeolites prepared by alkaline treatment are extensively discussed. It is expected that this approach will be useful for understanding how alkaline treatment acts on different hierarchical structures and will thus open doors to achieve other hierarchical zeolites by this method. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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23 pages, 1534 KiB  
Review
Homogeneous and Heterogeneous Catalytic Ozonation of Textile Wastewater: Application and Mechanism
by Magdalena Bilińska, Lucyna Bilińska and Marta Gmurek
Catalysts 2023, 13(1), 6; https://doi.org/10.3390/catal13010006 - 21 Dec 2022
Cited by 3 | Viewed by 2041
Abstract
This paper presents an overview of textile wastewater treatment by catalytic ozonation, highlighting the parameters of the process and accompanying mechanisms. Since more than 800,000 tons of dyes are produced annually and thousands of cubic meters of highly polluted textile wastewater have been [...] Read more.
This paper presents an overview of textile wastewater treatment by catalytic ozonation, highlighting the parameters of the process and accompanying mechanisms. Since more than 800,000 tons of dyes are produced annually and thousands of cubic meters of highly polluted textile wastewater have been emitted into the environment every day, this issue has become an environmental concern. Due to the high oxidative potential of ozone (2.08 V) and hydroxyl radical (2.80 V), the main reactive species in catalytic ozonation, the burdensome organic pollutants, including textile dyes, can be successfully decomposed. The paper shows the main groups of catalysts, emphasizing novel structural, nano-structured, and functionalized materials. The examples of catalytic ozonation in the industrial application for real textile wastewater were specially highlighted. Full article
(This article belongs to the Special Issue Microporous and Mesoporous Materials for Catalytic Applications)
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: Production of fine chemicals using microporous and mesoporous heterogeneous catalysts
Authors: Joseph Lantos; Narendra Kumar; Basudeb Saha
Affiliation: Laboratory of Industrial Chemistry and Reaction Engineering, Faculty of Science and Engineering, Johan Gadolin Proess Chemistry Centre, Åbo Akademi University, Henriksgatan 2, FI20500 Turku, Finland
Abstract: Fine chemicals are produced in small annual volume batch processes (often <10,000 tonnes per year), with a high associated price (usually > $10/kg). As a result of their usage in the production of speciality chemicals, in areas including agrochemicals, fragrances and pharmaceuticals, their necessity will remain high for the foreseeable future. This review article assesses current methods used to produce fine chemicals with heterogeneous catalysts, including both well-established methods as well as newer experimental methods. A wide range of methods utilising microporous and mesoporous catalysts has been explored, including their preparation and modification before use in industry. Their potential drawbacks, as well as benefits, have been analysed, with their feasibility compared to newer, recently emerging catalysts. The field of heterogeneous catalysis for fine chemical production is a dynamic and ever-changing area of research. This deeper insight into catalytic behaviour and material properties will produce more efficient, selective, and sustainable processes in the fine chemical industry. The findings from this article will provide an excellent foundation for further exploration and a critical review in this field of fine chemical production using micro- and mesoporous heterogeneous catalysts.

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