Microporous and Mesoporous Materials最新文献

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Construction of mesoporous carbon sphere with local short-range ordered graphitized structure for high-rate potassium storage 高速率储钾用局部短程有序石墨化介孔碳球的构建
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-23 DOI: 10.1016/j.micromeso.2025.113661
Yutong Zhao , Qian Chen , Hao Wang , Runguo Zheng , Zhishuang Song , Hongyu Sun , Zhiyuan Wang , Yanguo Liu
{"title":"Construction of mesoporous carbon sphere with local short-range ordered graphitized structure for high-rate potassium storage","authors":"Yutong Zhao ,&nbsp;Qian Chen ,&nbsp;Hao Wang ,&nbsp;Runguo Zheng ,&nbsp;Zhishuang Song ,&nbsp;Hongyu Sun ,&nbsp;Zhiyuan Wang ,&nbsp;Yanguo Liu","doi":"10.1016/j.micromeso.2025.113661","DOIUrl":"10.1016/j.micromeso.2025.113661","url":null,"abstract":"<div><div>Mesoporous carbon spheres (MCSs) have emerged as promising high-performance anodes of potassium ion batteries (PIBs) due to their larger layer spacing, randomly distributed amorphous regions, and abundance of defect sites. However, achieving high potassium-storage capacity at high current densities remains a difficult challenge due to its highly disordered structure leading to low conductivity. Herein, we propose a novel synthetic strategy to introduce locally short-range ordered graphitized structure into mesoporous carbon spheres to tunning the morphology and the internal structure, which improves the electrical conductivity, increases the specific surface area, and enriches K<sup>+</sup> intercalation sites. The optimized locally graphitized mesoporous carbon spheres (LGMCSs-2) exhibit a high-rate performance (210.1 mAh g<sup>−1</sup>) at 5 A g<sup>−1</sup> and delivers a capacity of 214.2 mAh g<sup>−1</sup> at 1 A g<sup>−1</sup> after 500 cycles. Even after 1000 cycles at 5 A g<sup>−1</sup>, it can still maintain a capacity of 144.3 mAh g<sup>−1</sup>. The superior rate capability and excellent cycling stability of LGMCSs-2 electrode are attributed to the well-defined mesoporous structure and locally graphitized structure design, which enhance the potassium-ion reaction kinetics. This work provides a new approach to designing local short-range ordered MCSs and offers valuable insights into the carbon-based anodes with fast charge/discharge capability for PIBs.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"394 ","pages":"Article 113661"},"PeriodicalIF":4.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143899606","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}
引用次数: 0
Preparation of mesoporous silica nanoparticles by spray drying 喷雾干燥法制备介孔二氧化硅纳米颗粒
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-22 DOI: 10.1016/j.micromeso.2025.113646
Lucía Gómez, Eva María Rivero-Buceta, Carla Vidaurre-Agut, Pablo Botella
{"title":"Preparation of mesoporous silica nanoparticles by spray drying","authors":"Lucía Gómez,&nbsp;Eva María Rivero-Buceta,&nbsp;Carla Vidaurre-Agut,&nbsp;Pablo Botella","doi":"10.1016/j.micromeso.2025.113646","DOIUrl":"10.1016/j.micromeso.2025.113646","url":null,"abstract":"<div><div>Mesoporous silica nanoparticles (MSNs) are usually obtained by conventional sol-gel synthesis techniques, in a process that requires long reaction periods, and goes through many critical steps. Small variation in the synthesis conditions can modify the morphology, structural and textural properties of materials. An alternative route for silica nanoparticles manufacturing is the spray drying (SD) technique, which involves particle formation by evaporation-induced hydrolysis and condensation of silicates, also providing continuous production. In this context, we have developed a new SD-based methodology for the preparation of well-dispersed MSNs by properly adjusting the pH of the synthesis mixture (e.g., pH = 8.5), and using NaF as silica mobilizing agent. These nanoparticles present wormhole-like pores that are randomly distributed in all directions and hexagonal symmetry easily recognizable in the mesoporous wall at small domains. In addition, optimizing the gas inlet temperature (T<sub>in</sub>) to 90 °C promoted rapid assembly between silicate network building species during the SD process, yielding nanoparticles with good structural and textural properties. This technique is highly scalable and adaptable to the industrial stage, showing enormous interest in the pharmaceutical development.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"393 ","pages":"Article 113646"},"PeriodicalIF":4.8,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143877120","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}
引用次数: 0
A strategy for synthesizing an ordered porous beta zeolite support for Ni2P catalysts with enhanced hydrodenitrogenation performance 一种具有增强加氢脱氮性能的有序多孔沸石载体Ni2P催化剂的合成策略
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-21 DOI: 10.1016/j.micromeso.2025.113651
Xiao Zhang , Yuan Zhuang , Shuqin Liang , Hanzhang Gong , Jian Liu
{"title":"A strategy for synthesizing an ordered porous beta zeolite support for Ni2P catalysts with enhanced hydrodenitrogenation performance","authors":"Xiao Zhang ,&nbsp;Yuan Zhuang ,&nbsp;Shuqin Liang ,&nbsp;Hanzhang Gong ,&nbsp;Jian Liu","doi":"10.1016/j.micromeso.2025.113651","DOIUrl":"10.1016/j.micromeso.2025.113651","url":null,"abstract":"<div><div>An ordered macroporous Beta zeolite (OMbeta) support was synthesized via a bottom-up templating strategy and used to prepare a highly active Ni<sub>2</sub>P (nickel phosphide) catalyst for hydrodenitrogenation (HDN). The formation mechanism of the ordered porous Beta zeolite was elucidated through detailed characterization. SEM images reveal that the Beta zeolite is composed of ∼250 nm spherical crystals, densely packed in an opal-like arrangement, with ∼55 nm voids forming between the crystallites due to shrinkage during synthesis. This interconnected microporous–macroporous structure significantly improves reactant diffusion and facilitates uniform Ni<sub>2</sub>P dispersion. As a result, the Ni<sub>2</sub>P/OMbeta catalyst exhibits enhanced quinoline HDN activity compared to Ni<sub>2</sub>P supported on conventional Beta zeolite.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"393 ","pages":"Article 113651"},"PeriodicalIF":4.8,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143870664","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}
引用次数: 0
γ-Aminobutyric acid-promoted crystallization of Beta zeolite and its application for direct amination of isobutene with ammonia γ-氨基丁酸促进β沸石结晶及其在氨直接胺化异丁烯中的应用
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-17 DOI: 10.1016/j.micromeso.2025.113648
Yijun Zhong , Dongpu Zhao , Weifeng Chu , Fucun Chen , Jie An , Yanan Wang , Wanling Shen , Shenglin Liu , Longya Xu
{"title":"γ-Aminobutyric acid-promoted crystallization of Beta zeolite and its application for direct amination of isobutene with ammonia","authors":"Yijun Zhong ,&nbsp;Dongpu Zhao ,&nbsp;Weifeng Chu ,&nbsp;Fucun Chen ,&nbsp;Jie An ,&nbsp;Yanan Wang ,&nbsp;Wanling Shen ,&nbsp;Shenglin Liu ,&nbsp;Longya Xu","doi":"10.1016/j.micromeso.2025.113648","DOIUrl":"10.1016/j.micromeso.2025.113648","url":null,"abstract":"<div><div>Beta zeolite is a significant catalyst used in petroleum refining and fine chemical course. We report a novel way to considerably shorten the crystallization time of Beta zeolite by adding γ-aminobutyric acid (GABA) as a ‘promoter’. The synthesis parameters are systematically investigated to unveil the promotion effect of GABA on Beta zeolite synthesis via a range of characterization skills, such as XRD, SEM, TEM, TG-DTG, NH<sub>3</sub>-TPD, Py-IR and NMR. The results demonstrate that under hydrothermal synthesis at 140 °C (initial Si/Al<sub>2</sub> = 43), the addition of GABA has been shown to result in a significant reduction in crystallization time, from 130 h to 18 h, while concurrently enhancing product yield from 51.7 % to 76.1 %. The resulting Si/Al<sub>2</sub> ratio increases from 22.6 to 33.1, suggesting that GABA regulates aluminum incorporation kinetics during zeolite nucleation. GABA can break the hydration layer round TEA<sup>+</sup> and aluminosilicate, and consequently, the formation of 5Rs structure and the nucleation process are accelerated. Meanwhile, the Hoffmann decomposition of TEAOH is inhibited as well. In comparison with the conventionally synthesized counterpart, the fast-synthesized Beta zeolite possessing high product yield and high Si/Al<sub>2</sub> ratio, exhibits comparable or even better catalytic performance in the direct amination of isobutene (<em>i</em>-C<sub>4</sub>H<sub>8</sub>) with ammonia (NH<sub>3</sub>), due to its relatively high concentration of weak acid site.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113648"},"PeriodicalIF":4.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850459","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}
引用次数: 0
Two-stage crystallisation of the MFI zeolite: kinetic control for efficient catalyst development MFI沸石的两阶段结晶:高效催化剂开发的动力学控制
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-17 DOI: 10.1016/j.micromeso.2025.113649
Vladimir S. Pavlov , Daniil V. Bruter , Andrey V. Efimov , Andrey G. Popov , Irina I. Ivanova , Vladimir L. Zholobenko
{"title":"Two-stage crystallisation of the MFI zeolite: kinetic control for efficient catalyst development","authors":"Vladimir S. Pavlov ,&nbsp;Daniil V. Bruter ,&nbsp;Andrey V. Efimov ,&nbsp;Andrey G. Popov ,&nbsp;Irina I. Ivanova ,&nbsp;Vladimir L. Zholobenko","doi":"10.1016/j.micromeso.2025.113649","DOIUrl":"10.1016/j.micromeso.2025.113649","url":null,"abstract":"<div><div>A detailed investigation of the MFI zeolite crystallisation mechanism in an alkaline synthetic gel system has been carried out using XRD, SEM, nitrogen adsorption, ammonia TPD, elemental analysis, NMR and FTIR spectroscopy. During the first stage of the synthesis, a highly crystalline zeolite is formed via solid hydrogel transformation mechanism, while for a prolonged synthesis, a second stage of crystallisation is clearly distinguished. The zeolite yield and its Si/Al ratio increase during the second stage, whereas the number of defect sites and the mesopore volume decrease. The second stage leads to increased diffusion limitations owing to the blockage of the transport mesopores and to shortened catalyst lifetime in the MTH and butenes oligomerisation processes as well as to a lower activity in toluene alkylation with methanol. Identification of the second stage of crystallisation potentially allows for fine tuning of the zeolite catalytic properties by varying the crystallisation time.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113649"},"PeriodicalIF":4.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850553","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}
引用次数: 0
Facile fabrication of hierarchical SAPO-34 zeolite with enhanced MTO catalytic performance 提高MTO催化性能的SAPO-34分子筛的简易制备
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-17 DOI: 10.1016/j.micromeso.2025.113647
Weijiong Dai, Zongqiang Liu, Jing Zhao, Yan Wang, Jiajun Zheng, Ruifeng Li
{"title":"Facile fabrication of hierarchical SAPO-34 zeolite with enhanced MTO catalytic performance","authors":"Weijiong Dai,&nbsp;Zongqiang Liu,&nbsp;Jing Zhao,&nbsp;Yan Wang,&nbsp;Jiajun Zheng,&nbsp;Ruifeng Li","doi":"10.1016/j.micromeso.2025.113647","DOIUrl":"10.1016/j.micromeso.2025.113647","url":null,"abstract":"<div><div>SAPO-34 zeolites with excellent selectivity towards to light olefins and highly catalytic stability are highly desirable. In this work, SAPO-34 zeolite (SAPO-34-S-F) featuring both significantly reduced crystal dimension and a hierarchical structure was synthesized for the first time through a seed-assisted strategy employing cost-effective triethylamine (TEA) as the only organic structure-directing agent (OSDA) in the NH<sub>4</sub>F-containing medium. The resulting SAPO-34 zeolite demonstrated exceptional catalytic performance in methanol-to-olefin (MTO) reaction, exhibiting a substantially increased catalytic lifetime of 525 min as well as an impressive light olefin selectivity of up to 83.7 %. These results significantly outperform those of conventional SAPO-34 zeolite with larger crystal dimension synthesized using TEA as OSDA, and SAPO-34 zeolite with similar crystal dimension synthesized without fluoride addition. Thermogravimetric analysis (TGA) of the spent catalysts revealed that SAPO-34-S-F possesses enhanced coke tolerance. Furthermore, in situ UV/Vis studies of the organic intermediates generated on zeolites during MTO reaction provided additional evidence for the excellent catalytic activity and stability of the SAPO-34-S-F sample. These findings offer important insights for the rational development of stable and high-efficiency SAPO-34 zeolite for MTO reaction.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113647"},"PeriodicalIF":4.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850460","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}
引用次数: 0
A rapid microwave-assisted solvothermal La3+ ion exchange of NaA zeolite membranes for enhanced performance of ethanol dehydration NaA沸石膜的快速微波辅助溶剂热La3+离子交换提高乙醇脱水性能
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-16 DOI: 10.1016/j.micromeso.2025.113645
Wenbin Zhao , Jinhuai Hua , Yi Cao , Rui Yao , Yanshuo Li
{"title":"A rapid microwave-assisted solvothermal La3+ ion exchange of NaA zeolite membranes for enhanced performance of ethanol dehydration","authors":"Wenbin Zhao ,&nbsp;Jinhuai Hua ,&nbsp;Yi Cao ,&nbsp;Rui Yao ,&nbsp;Yanshuo Li","doi":"10.1016/j.micromeso.2025.113645","DOIUrl":"10.1016/j.micromeso.2025.113645","url":null,"abstract":"<div><div>A microwave-assisted solvothermal method was developed to achieve La<sup>3+</sup> exchange in NaA zeolite membranes for enhanced ethanol dehydration via pervaporation. Traditional ion-exchange processes are time-consuming and risk structural degradation, whereas the proposed approach utilizes alcohol-based solvents under microwave irradiation to accelerate ion exchange while preserving membrane integrity. By optimizing solvent selection (isopropanol) and La<sup>3+</sup> concentration (0.04–0.05 mol L<sup>−1</sup>), the modified La-LTA membrane exhibited simultaneous improvements in water flux (up to 12.78 % increase) and separation factor (up to 227 % enhancement), particularly in low-water-content systems. Characterization via SEM, XRD, and XPS confirmed retained crystallinity and successful La<sup>3+</sup> incorporation (35.42 % exchange degree). The method's universality was validated by exchanging other ions (Li<sup>+</sup>, Cu<sup>2+</sup>, Nd<sup>3+</sup>), with Li-LTA and Nd-LTA membranes also showing dual performance enhancements. This work provides an energy-efficient, scalable strategy to tailor zeolite membranes for industrial dehydration applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113645"},"PeriodicalIF":4.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143850461","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}
引用次数: 0
Adsorption separation of propylene/propane by pressure induced flexible porous MOF 压力诱导柔性多孔MOF吸附分离丙烯/丙烷
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-16 DOI: 10.1016/j.micromeso.2025.113644
Huiping Chen , Meiling Li , Dongxu Gu , Guang Che
{"title":"Adsorption separation of propylene/propane by pressure induced flexible porous MOF","authors":"Huiping Chen ,&nbsp;Meiling Li ,&nbsp;Dongxu Gu ,&nbsp;Guang Che","doi":"10.1016/j.micromeso.2025.113644","DOIUrl":"10.1016/j.micromeso.2025.113644","url":null,"abstract":"<div><div>The separation of C<sub>3</sub>H<sub>6</sub> from C<sub>3</sub>H<sub>8</sub> represents a significant yet challenging industrial task. Utilizing adsorption separation technology based on porous materials emerges as an energy-saving and cost-effective strategy. In this study, we investigate a flexible porous MOF, HNU-49, as a promising adsorbent for the efficient separation of C<sub>3</sub>H<sub>6</sub> and C<sub>3</sub>H<sub>8</sub> within the temperature range of 288–308 K. Due to its adaptable microporous structure, HNU-49 displays a distinct guest-dependent pressure-induced gate-opening effect, facilitating the effective separation of propylene and propane. Experimental studies, including adsorption isotherms and transient breakthrough experiments, were conducted to evaluate the separation performance of HNU-49, and cyclic experiments were performed to assess its structural stability. At a temperature of 298 K and a pressure of 0.2 bar, HNU-49 exhibits an IAST selectivity of 5.13 for C<sub>3</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>8</sub>. The findings indicate that flexible MOFs with guest-dependent pressure-induced gate-opening effects hold potential applications in selective gas adsorption and separation. Moreover, these stable materials demonstrate good regenerability, making them advantageous for practical applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"393 ","pages":"Article 113644"},"PeriodicalIF":4.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854783","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}
引用次数: 0
Mesolite, |Na2Ca2(H2O)8|[Al6Si9O30]: Crystal structure reinvestigation and pressure-mediated crystal-fluid interaction Mesolite, |Na2Ca2(H2O)8|[Al6Si9O30]:晶体结构再研究与压力介导的晶体-流体相互作用
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-15 DOI: 10.1016/j.micromeso.2025.113643
Tommaso Battiston , Davide Comboni , Paolo Lotti , Benedetta Chrappan-Soldavini , Oscar Fabelo , Laura Canadillas-Delgado , Gaston Garbarino , Hanns-Peter Liermann , G. Diego Gatta
{"title":"Mesolite, |Na2Ca2(H2O)8|[Al6Si9O30]: Crystal structure reinvestigation and pressure-mediated crystal-fluid interaction","authors":"Tommaso Battiston ,&nbsp;Davide Comboni ,&nbsp;Paolo Lotti ,&nbsp;Benedetta Chrappan-Soldavini ,&nbsp;Oscar Fabelo ,&nbsp;Laura Canadillas-Delgado ,&nbsp;Gaston Garbarino ,&nbsp;Hanns-Peter Liermann ,&nbsp;G. Diego Gatta","doi":"10.1016/j.micromeso.2025.113643","DOIUrl":"10.1016/j.micromeso.2025.113643","url":null,"abstract":"<div><div>The crystal structure and the pressure-mediated crystal-fluid interaction of mesolite have been re-investigated by a multi-methodological approach, based on single-crystal neutron diffraction and by <em>in-situ</em> single-crystal synchrotron X-ray diffraction, using a diamond anvil cell. The structure refinement based on neutron intensity data collected at 20 K confirms the general model previously reported for mesolite, but largely improves the description of the hydrogen-bond network (with accurate sites location, their libration regime and interactions). Twelve out of the nineteen oxygen sites in the crystal structure of mesolite are involved in H-bonds as <em>donors</em> or as <em>acceptors</em>, reflecting the complex configuration of the H-bonding network. In the high-pressure investigations, four different pressure-transmitting fluids have been employed: the non-penetrating <em>Daphne oil</em> 7575 and the potentially penetrating methanol:ethanol:H<sub>2</sub>O (1:1:1) mixture, distilled H<sub>2</sub>O and liquid Ne. The <em>Daphne oil</em> 7575 experiment provided insight into the intrinsic compressional behaviour of mesolite, without any pressure-induced crystal-fluid interaction, yielding an isothermal bulk modulus <em>K</em><sub><em>V0</em></sub> = 55.9(7) GPa (<em>β</em><sub><em>V0</em></sub> = 0.0179(2) GPa<sup>−1</sup>). In the aqueous mixtures, H<sub>2</sub>O molecules have been observed to continuously penetrate into the structural cavities, firstly in the natrolite- and then in the scolecite-type sheets, in the pressure range 0.8–1.9 GPa. By comparing the results of this study to the literature data, there is an apparent correlation between the pressure at which the adsorption process occurs and the H<sub>2</sub>O concentration of the pressure-transmitting medium: a higher H<sub>2</sub>O fraction allows the over-hydration of the scolecite-type sheets at lower pressures. When compressed in liquid Ne, atoms of neon appear to be able to penetrate into the natrolite-type sheets, interacting with the extra-framework population <em>via</em> weak van der Waals forces.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"393 ","pages":"Article 113643"},"PeriodicalIF":4.8,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143877121","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}
引用次数: 0
Enhancement of the olefin selectivity over ZnSAPO-34 zeolite toward methanol-to-olefins conversion and its mechanistic interpretation ZnSAPO-34 沸石对甲醇-烯烃转化的烯烃选择性增强及其机理解释
IF 4.8 3区 材料科学
Microporous and Mesoporous Materials Pub Date : 2025-04-12 DOI: 10.1016/j.micromeso.2025.113632
Chang Wang , Lei Zhang , Jiahui Yang , Jun Yu , Xue Shao , Lina Zhang , Runze Liu , Weiping Zhu , Weili Dai
{"title":"Enhancement of the olefin selectivity over ZnSAPO-34 zeolite toward methanol-to-olefins conversion and its mechanistic interpretation","authors":"Chang Wang ,&nbsp;Lei Zhang ,&nbsp;Jiahui Yang ,&nbsp;Jun Yu ,&nbsp;Xue Shao ,&nbsp;Lina Zhang ,&nbsp;Runze Liu ,&nbsp;Weiping Zhu ,&nbsp;Weili Dai","doi":"10.1016/j.micromeso.2025.113632","DOIUrl":"10.1016/j.micromeso.2025.113632","url":null,"abstract":"<div><div>The SAPO-34 zeolite serves as a crucial catalyst in the methanol-to-olefins (MTO) conversion to produce ethylene and propylene, yet suffering from the unsatisfied trade-off between long catalyst lifetime and high light olefins selectivity. Herein, we report a stable and efficient hierarchical ZnSAPO-34 zeolite prepared via hydrothermal method, which is featured with the successful introduction of Zn species into SAPO-34 framework. Impressively, the ZnSAPO-34 catalyst achieves a significantly enhanced ethylene selectivity of 60 % without obviously sacrificing catalyst lifetime. A combination study including online mass spectrometer (MS), <sup>13</sup>C MAS NMR and <em>in situ</em> UV–visible (UV–vis) spectroscopy demonstrates that Zn species facilitate the initial generation of carbonyl species accompanied by the formation of hydrocarbon pool species, thus boosting the ethylene selectivity via the aromatic-based cycle. Meanwhile, the one-step introduction of Zn species leads to smaller crystal size and increases mesoporous in zeolite, enhancing the diffusion capacity of the ZnSAPO-34 sample, which accounts for the almost unchanged catalyst lifetime. The mechanistic interpretation provides a novel perspective to optimize zeolite catalysts by one-step introducing heteroatom, which shows potential applications in industrial MTO production.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113632"},"PeriodicalIF":4.8,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143829345","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}
引用次数: 0
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