Hafez Maghsoudi, Mohammad Azadi Tabar, Mohsen Gholami, Joeri F.M. Denayer
{"title":"Maximizing methane production in adsorptive nitrogen removal from natural gas: The impact of dehydration temperature on Ba-ETS-4 separation performance","authors":"Hafez Maghsoudi, Mohammad Azadi Tabar, Mohsen Gholami, Joeri F.M. Denayer","doi":"10.1016/j.micromeso.2024.113375","DOIUrl":"10.1016/j.micromeso.2024.113375","url":null,"abstract":"<div><div>Ba-ETS-4 is a promising adsorbent for nitrogen removal from low-grade natural gas. However, the Ba-ETS-4 adsorption characteristics, i.e., both adsorption kinetics and equilibrium capacity, change by dehydration temperature owing to structural shrinkage and pore contraction which finally impact the separation performance of the adsorption bed. In this paper, experimental breakthrough data are provided for N<sub>2</sub>/CH<sub>4</sub> separation at various Ba-ETS-4 dehydration temperatures (250°C-450 °C) followed by a separation performance analysis in generating methane as the main product. Additionally, isotherm data at different temperatures (20 °C, 40 °C, 60 °C and 80 °C) are presented for selected dehydration temperatures (250 °C, 350 °C, 400 °C and 440 °C). The results revealed that an increase in dehydration temperature leads to a decrease in adsorption capacity but a better separation by providing more hindrance for CH<sub>4</sub> diffusion, while not affecting the N<sub>2</sub> breakthrough wavefront. At a dehydration temperature of 250 °C, the N<sub>2</sub> breakthrough time is the highest, indicating the ability to process a larger feed. However, this also leads to the least CH<sub>4</sub> production (0.037 mmol/g), as most of the fed CH<sub>4</sub> is adsorbed onto the bed. Interestingly, an increase in dehydration temperature leads to an increase in CH<sub>4</sub> production up to 420 °C (0.140 mmol/g), after which the CH<sub>4</sub> production decreases sharply.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113375"},"PeriodicalIF":4.8,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marieke van Leeuwen , Nina Plankensteiner , Rahul Maity , Jesus Gandara Loe , Joeri F.M. Denayer , Rob Ameloot , Philippe M. Vereecken
{"title":"Surface-enhanced CO2 capture in ionic liquid-silica nanocomposites via sol-gel synthesis in the low partial pressure range","authors":"Marieke van Leeuwen , Nina Plankensteiner , Rahul Maity , Jesus Gandara Loe , Joeri F.M. Denayer , Rob Ameloot , Philippe M. Vereecken","doi":"10.1016/j.micromeso.2024.113374","DOIUrl":"10.1016/j.micromeso.2024.113374","url":null,"abstract":"<div><div>Ionic liquid-containing silica nanocomposites enable the capture of carbon dioxide from gas mixtures containing nitrogen, oxygen, and methane. Synthesis methods explored for such nanocomposites include impregnating porous silica and one-pot synthesis via a sol-gel process. This research investigates a non-hydrolytic sol-gel route for nanocomposite materials enabling CO<sub>2</sub> capture at low partial pressures (0.1–0.4 bar). The tetraethyl orthosilicate (TEOS) precursor condensation resulted in a silica matrix formed around ionic liquid domains, for bis(trifluorosulfonylimide) (TFSI<sup>−</sup>)-based ionic liquids with 1-butyl-1-methylpyrrolidinium (BMP<sup>+</sup>), 1-butyl-3-methylimidazolium (BMI<sup>+</sup>), 1-ethyl-3-methylimidazolium (EMI<sup>+</sup>) and 1-hexyl-3-methylimidazolium (HMI<sup>+</sup>) cations. Using a one-pot synthesis method enables exploring CO<sub>2</sub> sorption in such nanocomposites for ionic liquid-to-silica contents up to fourteen times higher than in previously reported studies. Moreover, the selected synthesis method provides greater tunability in deposition methods and their control. The silica host matrix was characterized by N<sub>2</sub> adsorption isotherms at 77 K after solvent extraction and supercritical drying of the material for ionic liquid removal. The pore size distribution of the freestanding silica network was observed via Scanning Electron Microscope (SEM) imaging and assessed with the Barrett-Joyner-Halenda (BJH) method for nanocomposites of different [BMP][TFSI]-to-silica ratio. The CO<sub>2</sub> uptake at pressures down to 0.1 bar was evaluated from CO<sub>2</sub> adsorption isotherms at 303 K. The confinement of [BMP][TFSI] resulted in a beneficial effect for the CO<sub>2</sub> uptake at lower partial pressures, with an uptake five times higher than the sum of the individual uptake expected from the contained ionic liquid and silica. The reported results show the advantage of a one-pot synthesis method for broader tunability of the nanocomposite, both regarding its content and application, as well as increased performance at lower partial pressures compared to the nanocomposite's individual constituents.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113374"},"PeriodicalIF":4.8,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527441","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jéssica de Lara Andrade , Angélica Gonçalves de Oliveira , Cezar Augusto Moreira , Carlos Eduardo Scanferla , Sandro Marcio Lima , Luis Humberto da Cunha Andrade , Paulo Rodrigo Stival Bittencourt , Daniela Martins Fernandes de Oliveira
{"title":"Multifunctional nanoplatforms based on alumina-coated mesoporous silica with potential for cancer theranostics applications","authors":"Jéssica de Lara Andrade , Angélica Gonçalves de Oliveira , Cezar Augusto Moreira , Carlos Eduardo Scanferla , Sandro Marcio Lima , Luis Humberto da Cunha Andrade , Paulo Rodrigo Stival Bittencourt , Daniela Martins Fernandes de Oliveira","doi":"10.1016/j.micromeso.2024.113373","DOIUrl":"10.1016/j.micromeso.2024.113373","url":null,"abstract":"<div><div>Multifunctional nanoplatforms based on mesoporous silica coated with alumina were successfully and sustainably synthesized using sodium silicate extracted from rice husk ash (RHA), demonstrating the potential for cancer theranostics. The hybrid nanostructures produced (C2-600 and C4-600) from two different calcination times exhibited distinct morphologies, textural parameters, and degrees of mesoscopic organization. As expected, the Al<sub>2</sub>O<sub>3</sub> coating on the mesoporous silica nanoparticles (MSNs) reduced the specific surface area from 720 m<sup>2</sup>/g to 122 m<sup>2</sup>/g (C2-600) and 57 m<sup>2</sup>/g (C4-600), while preserving their mesoporous structure. Additionally, both C2-600 and C4-600 showed relatively good stability across a wide pH interval, with a zeta potential of ζ = −15 mV and hydrodynamic diameter (D<sub>h</sub>) ranging from 160 to 670 nm, depending on the pH of the medium. These peculiar characteristics resulted in high encapsulation efficiency (EE ≈ 90 %) for the doxorubicin (DOX) anticancer drug, as well as sustained drug release in simulated gastric fluid (SGF, pH 1.2) and simulated intestinal fluid (SIF, pH 7.4). Appreciably, C4-600-DOX released approximately 83 % of the drug over 96 h and demonstrated significant biodegradation in simulated biological media. Furthermore, the hybrid nanoplatforms exhibited strong optical absorption between 250 and 420 nm, along with broad and intense photoluminescence (PL) in the near-infrared (NIR) region (680–900 nm), which is highly desirable for NIR-fluorescence diagnostic imaging. Notably, the hybrid nanoplatforms without DOX were non-cytotoxic to fibroblast and Caco-2 cells, while the DOX-loaded nanoplatforms exhibited selectivity and potent anticancer activity, inhibiting approximately 80 % of Caco-2 colorectal cancer cells after 72 h. These findings demonstrate that C2-600 and C4-600 are innovative, multifunctional and biodegradable nanoplatforms with powerful potential as drug carriers and fluorescence imaging agents, making them promising candidates for cancer theranostics.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113373"},"PeriodicalIF":4.8,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Vera V. Butova , Videlina R. Zdravkova , Olga A. Burachevskaia , Ivan E. Gorban , Mikhail A. Soldatov , Konstantin I. Hadjiivanov
{"title":"FTIR traced modification of defect-engineered UiO-66 for enhanced accessibility of zirconium sites","authors":"Vera V. Butova , Videlina R. Zdravkova , Olga A. Burachevskaia , Ivan E. Gorban , Mikhail A. Soldatov , Konstantin I. Hadjiivanov","doi":"10.1016/j.micromeso.2024.113372","DOIUrl":"10.1016/j.micromeso.2024.113372","url":null,"abstract":"<div><div>This research focuses on identifying the accessibility of active sites within the defect-engineered UiO-66 framework. The task is particularly challenging due to reversible changes in the framework during dehydroxylation: the loss of μ<sub>3</sub>-OH groups with simultaneous reduction of the Zr coordination number and the possible creation of Zr<sup>4+</sup> Lewis acid sites in defect MOFs. We used in-situ FTIR and XANES analyses, as well as interaction with probe molecules, to monitor the changes in Zr coordination and the host-guest interaction. The defects were introduced using benzoic acid as a modulator, which coordinated to Zr<sup>4+</sup> in defective pores. Our results showed that the UiO-66 sample synthesized with benzoic acid contained defects, but these were concealed under benzoate residues and thus inaccessible. Standard washing and heating did not remove benzoate anions. Dehydroxylation of the sample leads to the development of “hidden” Lewis acidity: some Zr<sup>4+</sup> sites were not able to form complexes with the weak base CO, but they interact with the stronger bases acetonitrile. Additionally, in-situ XANES analysis revealed that the effect of acetonitrile adsorption is similar to that of water rehydration. Treatment of the sample with HCl and DMF led to the replacement of benzoates with formate ions, exposing the bare Zr<sup>4+</sup> sites within the defective pores. These cationic sites acted as true Lewis acids and were able to coordinate both CO and acetonitrile. Our findings emphasize that the active sites in UiO-66 highly depend on synthesis conditions and post-synthetic treatments. Comprehensive site-specific methods are crucial for accurately predicting and identifying these active sites.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113372"},"PeriodicalIF":4.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Application of aluminosilicate residue-based zeolite from lithium extraction in water treatment","authors":"Fatima Ibsaine , Justine Dionne , Lan Huong Tran , Lucie Coudert , Louis-César Pasquier , Jean-François Blais","doi":"10.1016/j.micromeso.2024.113370","DOIUrl":"10.1016/j.micromeso.2024.113370","url":null,"abstract":"<div><div>In a previous study, the Na-P1 type zeolites were synthesized from aluminosilicate residues using an efficient and cost-effective process, exhibiting an excellent adsorption capacity for Ca<sup>2+</sup> in comparison to commercial zeolites 13X and A. Building upon this, the current study evaluates their performance for the adsorption of various elements, including Ca<sup>2+</sup>, Mg<sup>2+</sup>, and NH<sub>4</sub><sup>+</sup>. The objective was to evaluate the performance of the Na-P1 type zeolites for the adsorption of various elements, including Ca<sup>2+</sup>, Mg<sup>2+</sup>, and rare earth elements, with a particular emphasis on the adsorption kinetics and water hardness removal in comparison to commercial zeolite A. The results demonstrated that the Na-P1 zeolite exhibited a satisfactory sorption capacity for Ca<sup>2+</sup> and NH<sub>4</sub><sup>+</sup> ions (66 mg/g), while displaying a relatively lower effectiveness for the sorption of Mg<sup>2+</sup> ions (5.6 mg/g). The Langmuir model is particularly well suited to the sorption of Ca<sup>2+</sup>, while the Freundlich model is more appropriate for Mg<sup>2+</sup>. Both models demonstrated satisfactory representation of NH₄ ⁺ sorption. Moreover, the pseudo-second-order kinetic model provides an excellent description of the Ca<sup>2</sup>⁺ and Mg<sup>2</sup>⁺ sorption processes, while both models effectively describe the NH₄⁺ adsorption kinetics. Additionally, Na-P1 zeolite was observed to effectively reduce water hardness from 322 to 63 mg CaCO₃/L at temperatures of 10, 20, and 38 °C, and to 18 mg/L at 58 °C. These findings suggest that Na-P1 zeolite has promising potential for applications as a water softening agent. Regarding metals and rare earths, the Na-P1 zeolite demonstrated noteworthy sorption efficiencies for Cd<sup>2+</sup> (138 mg/g), Ce<sup>3+</sup> (209 mg/g), Cr<sup>3+</sup> (56.2 mg/g), and Cu<sup>2+</sup> (60.5 mg/g). However, it demonstrated lower sorption efficiencies for Co<sup>2+</sup>, Mn<sup>2+</sup>, Ni<sup>2+</sup> and Dy<sup>3+</sup> (below 16 mg/g). The findings illustrate that Na-P1 zeolites are effective for the adsorption of diverse elements, offering a promising avenue for the sustainable transformation of industrial waste into valuable materials for environmental applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113370"},"PeriodicalIF":4.8,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142438472","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Thai Q. Bui , Tomas Pokorny , Petr Machac , Zdenek Moravec , Eva Domincova Bergerova , Ales Styskalik
{"title":"Non-hydrolytic sol-gel synthesis of amine-functionalized silica: Template- and catalyst-free preparation of mesoporous catalysts for CO2 valorization","authors":"Thai Q. Bui , Tomas Pokorny , Petr Machac , Zdenek Moravec , Eva Domincova Bergerova , Ales Styskalik","doi":"10.1016/j.micromeso.2024.113371","DOIUrl":"10.1016/j.micromeso.2024.113371","url":null,"abstract":"<div><div>Carbon dioxide utilization presents an important and topical research topic. However, the performance of catalysts needed for CO<sub>2</sub> transformations does not achieve the necessary levels for their widespread application. To this end, we decided to study non-aqueous condensations providing amine-functionalized silica catalysts, possibly active in CO<sub>2</sub>-epoxide cycloaddition reaction. While non-hydrolytic sol-gel method is well-known for its efficiency in providing highly porous Lewis and Brønsted acid metallosilicates, here we show for the first time its application for the preparation of silica-based catalysts containing basic groups. First, the reaction conditions were screened to reproducibly obtain porous materials with preserved amine moieties. These were identified as follows: silicon tetraacetate and bridging tertiary amine silanes as precursors, toluene as a solvent, and temperature between 160 and 180 °C. In such a way, materials with up to 776 m<sup>2</sup> g<sup>−1</sup> and 1.58 cm<sup>3</sup> g<sup>−1</sup> were obtained in one-step process, without any template, after conventional drying step. Next, the amine-functionalized materials were tested in CO<sub>2</sub>-epoxide coupling providing cyclic organic carbonates with high selectivity (>99 %) and moderate activity (up to 86 % epichlorohydrin conversion after 1 h at 120 °C and 10 bar CO<sub>2</sub>). The characterization of spent catalysts revealed a presence of cyclic organic carbonates at the catalyst surface as well as conversion of tertiary amine groups to quaternary ammonium moieties.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113371"},"PeriodicalIF":4.8,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142446914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Study of metal sequenced spray impregnation method towards Co-Mo/γ-Al2O3 catalytic performance in hydrotreating of used coconut oil to liquid biohydrocarbon","authors":"Meissha Ayu Ardini , Triyono , Takayoshi Hara , Nobuyuki Ichikuni , Wega Trisunaryanti","doi":"10.1016/j.micromeso.2024.113357","DOIUrl":"10.1016/j.micromeso.2024.113357","url":null,"abstract":"<div><div>A series of bifunctional catalyst CoMo on γ-Al<sub>2</sub>O<sub>3</sub> have been successfully prepared using the spray impregnation (dry impregnation), with the variation in the metal sequence (Co-Mo and Mo-Co) and metal impregnation time gap (1-h, 24-h, and simultaneous). XRF indicated that the developed method causes a minimal amount of metal loss during the impregnation process. XRD shows that 24-h treatment reduces crystallinity compared to the 1-h and simultaneous catalysts. Co and Mo existed as CoAl<sub>2</sub>O<sub>4</sub>, CoO, and MoO<sub>3</sub> as reported by XANES and XPS. The preparation technique signified the catalyst's acidity and surface area. The Co-Mo/γ-Al<sub>2</sub>O<sub>3</sub> 24H has a high surface area (118.32 m<sup>2</sup> g<sup>−1</sup>), with a pore volume of 0.22 cm<sup>3</sup> g<sup>−1</sup>, and a pore diameter of 7.48 nm. It has a high proportion of weak acid sites (41.32 %) which is crucial to perform HDO reactions. Co-Mo/γ-Al<sub>2</sub>O<sub>3</sub> 24H showed high catalytic activity (40.32 wt% liquid product) and selectivity (85.61 % of biogasoline and 9.75 % of diesel fractions) from the hydrotreatment. Kimi@UGM2010.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113357"},"PeriodicalIF":4.8,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Direct synthesis of low-silica ZSM-48 zeolite via seed-assisted hydrothermal synthesis with 1,6-hexanediamine as template","authors":"Shiao Gao , Ahui Ma , Zhennan Yang, Sida Ge, Zhuwen Zhang, Zhijie Wu","doi":"10.1016/j.micromeso.2024.113369","DOIUrl":"10.1016/j.micromeso.2024.113369","url":null,"abstract":"<div><div>ZSM-48 zeolite is characteristic of 10-member ring (10-MR) one-dimensional tubular channel structure and finds extensive applications in catalytic hydroisomerization reactions. Here we developed an efficient synthetic strategy for low-silica ZSM-48 zeolite with a SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratio at 30–176 via a seed-assisted hydrothermal synthesis method, overcoming the limit that 1,6-hexanediamine (HDA) template can only be used to synthesize high-silica (i.e., SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratio >200) zeolites. A two-step crystallization procedure coupled with zeolite seed-assisted synthesis strategy was enrolled to realize well crystallized ZSM-48 zeolites, in which the zeolite nuclei are sufficiently produced at the nucleation temperature at 100 °C for 24 h with the aid of zeolite seeds, and the zeolite growth is proceeded at the crystallization temperature at 160 °C for 48 h. The morphology and particle size of low-silica ZSM-48 zeolite have been manipulated by adjusting the synthetic parameters, such as the alkalinity and silicon source of aluminosilicate gel for zeolite, the crystallization manner (static or dynamic crystallization), as well as the presence of additive (i.e., sodium chloride). The as-synthesized ZSM-48 zeolite possesses a high acid content of 0.194 mmol/g, highlighting its potential as an excellent acidic support for hydroisomerization catalysts. The cost-effective and environmentally friendly synthesis strategy, which is anticipated to expand the application of alkylamine organic templates in the synthesis of low-silica ZSM-48 zeolite.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"382 ","pages":"Article 113369"},"PeriodicalIF":4.8,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142527371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Controllable assembly of NiMo nano-wool shell on zeolite Y and its advanced behavior of hydrodesulfurization toward dibenzothiophene","authors":"Xiaoqian Li , Shenyong Ren , Lu Liu, Chi Yang","doi":"10.1016/j.micromeso.2024.113368","DOIUrl":"10.1016/j.micromeso.2024.113368","url":null,"abstract":"<div><div>A core-shell structured USY-xTT@NiMo catalyst was prepared through thermal treatment method and evaluated for the catalytic hydrodesulfurization (HDS) performance toward dibenzothiophene (DBT). The shell assembled from NiMoS nano-wool provided abundant active site. This nano-wool morphology and core-shell structure resulted in the catalyst with enhanced specific surface area, pore volume, lower interaction between the support and active metals, and facilitated metal dispersion. In addition, the nano-wool morphology and core-shell structure also promoted the degree of sulfurization and provided more sulfur vacancies, which enhanced the HDS performance of the corresponding catalysts. An efficient USY-16TT@NiMo catalyst with shorter slab lengths (average 2.50 nm), higher average stacking number (3.37 layers), and more edge active sites was assembled, which showed superior k<sub>HDS</sub> value of DBT up to 8.29 × 10<sup>−4</sup> mol g<sup>−1</sup> h<sup>−1</sup> and high direct desulfurization selectivity to be 88 %.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113368"},"PeriodicalIF":4.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142441277","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yue-lun Wang , Han-bing Gao , Wei-hua Zhao , Xu Yan , Jing Liang , Yun-Peng Zhao , Jing-pei Cao , Lin-jun Zhu
{"title":"Catalytic upgrading of lignite pyrolysis volatiles to light aromatics under methanol atmosphere over Zr and/or Fe modified hollow ZSM-5 zeolites","authors":"Yue-lun Wang , Han-bing Gao , Wei-hua Zhao , Xu Yan , Jing Liang , Yun-Peng Zhao , Jing-pei Cao , Lin-jun Zhu","doi":"10.1016/j.micromeso.2024.113362","DOIUrl":"10.1016/j.micromeso.2024.113362","url":null,"abstract":"<div><div>Fe and Zr modified hollow ZSM-5 zeolites were prepared and their applications in upgrading of lignite pyrolysis volatiles coupling with methanol to light aromatics were investigated. The results demonstrated that hollow zeolites with larger voids and shorter diffusion length favored the production of light aromatics. Adding Fe and Zr into ZSM-5 zeolites further enhanced BTX yields due to the synergism between metals and acid sites for promoting hydrodeoxygenation reactions. Meanwhile, Zr-Fe/HZ-5 catalyst with increasing Lewis acid sites facilitated methylation leading to high selectivity of xylene under methanol atmosphere. Moreover, diffusion behaviors of xylene were quantified. Higher self-diffusion coefficient of molecules in hollow zeolites led to the formation of less coke, while the incorporation of Fe and Zr promoted the formation of catalytic coke due to the increase of alkylation resulting in partial conversion of BTX into PAHs on external surfaces although the total coke yields were further decreased.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113362"},"PeriodicalIF":4.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}