Microporous and Mesoporous Materials最新文献

{"title":"Cu-trimesate and mesoporous silica composite as adsorbent showing enhanced CO2/CH4 and CO2/N2 selectivity for biogas and flue gas separation","authors":"Suman Dalakoti ,&nbsp;Narendra Singh ,&nbsp;Anjali Sharma ,&nbsp;Anjali Singh ,&nbsp;Madhur Sachdeva ,&nbsp;Swapnil Divekar ,&nbsp;Aarti Arya ,&nbsp;R. Surya Murali ,&nbsp;Soumen Dasgupta","doi":"10.1016/j.micromeso.2024.113354","DOIUrl":"10.1016/j.micromeso.2024.113354","url":null,"abstract":"<div><div>Due to their diverse structure, high porosity, and tunable functionality, Metal-Organic Frameworks (MOFs) hold great potential as materials for diverse applications, including gas separation. Material science researchers are focusing on creating flexible materials that have special properties. Most of the latest research mainly concentrates on fabricating composite materials of MOFs and other functional materials. These MOF-based composites can mitigate the limitations of pure MOFs and may even perform better than the individual components. Here, we present a systematic study on the effect of solvent in synthesising a composite (Cu-BTC@SBA-15) of Cu-trimesate MOF (aka CuBTC) and ordered mesoporous silica SBA-15, showing considerable improvement in selectivity for CO₂ adsorption from the flue gas and biogas. The pristine Cu-BTC, SBA-15 and the composites with different content of Cu-BTC were characterized by PXRD, BET, FT-IR, SEM, TEM and TGA techniques. The pure gas adsorption isotherms were measured for CO₂, CH₄, and N₂ gases. Ideal Adsorbed Solution Theory (IAST) is used for the binary selectivity calculations for gas systems such as CO₂/CH₄ and CO₂/N₂ in the context of biogas and flue gas separation. The composite exhibited an increase in CO₂/CH₄ selectivity by 39 % compared to pure Cu-BTC and 85 % compared to pure SBA-15. For the CO₂/N₂ system, the composite showed 38 % higher selectivity than Cu-BTC. The work has significance in the design of effective MOF-based composites for CO₂ separation. Our work might open up a new route to design multifunctional materials for worldwide applications through an adsorptive and or mixed matrix membrane route.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113354"},"PeriodicalIF":4.8,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142421418","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":"One-pot synthesis of Ir subnanosized clusters supported on MWW nanosheets as effective catalysts for C-C bond hydrogenolysis","authors":"Evgeny Naranov ,&nbsp;Alexey Sadovnikov ,&nbsp;Olga Arapova ,&nbsp;Dmitry Gorbunov ,&nbsp;Alexander Gorbunov ,&nbsp;Svetlana Shapovalova ,&nbsp;Alexander Guda ,&nbsp;Alexander Soldatov ,&nbsp;Anton Maximov","doi":"10.1016/j.micromeso.2024.113356","DOIUrl":"10.1016/j.micromeso.2024.113356","url":null,"abstract":"<div><div>The rational design synthesis of metal catalysts with high dispersion and ordered structure is a challenging subject in materials chemistry and heterogeneous catalysis. In this study, we report one-pot synthesis of Ir subnanosized particles supported on MWW nanosheets and their application in hydrogenolysis of decalin. Here, it has been found that C-C bond cleavage occurs <em>via</em> a synergistic carbocation and carbene mechanism on Ir-containing catalysts, and <em>via</em> carbocation in the case of solid acids. The combination of optimal acidic and metallic site characteristics in the subnanosized Ir supported on MWW nanosheets Pill_Ir-ZN_150 sample contributes to the high activity of the final catalysts. We expect that these Ir catalytic systems will open up more opportunities for hydrogenolysis of naphthenics to high-value products.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113356"},"PeriodicalIF":4.8,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142421424","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":"Imparting functionality into porphyrin metal–organic framework aerogels with uniform distributions for diversified applications","authors":"Yujun Wang ,&nbsp;Peng Zhang ,&nbsp;Chuantao Hou","doi":"10.1016/j.micromeso.2024.113355","DOIUrl":"10.1016/j.micromeso.2024.113355","url":null,"abstract":"<div><div>The incorporation of various functional nanoentities into pure metal–organic framework (MOF) aerogels can not only introduce additional functionality but also expands the application scenarios of MOF aerogels. Herein, a general and simple strategy for uniform incorporation of various functional nanomaterials into a porphyrin MOF aerogel is presented. Specifically, this strategy primarily involves the introduction of a surfactant polyvinylpyrrolidone (PVP) to disperse the nanomaterials in lipophilic solvents, followed by a direct solvothermal reaction with the precursors of the porphyrin MOF aerogel. Additionally, uniform aerogel composites consisting of two MOF components have also been developed by careful optimizing the reaction conditions. The resulting nanoentity@MOF aerogel composites exhibit positive properties that stem from the synergistic effects between the nanoentities and MOF aerogel, offering advanced applications in areas such as photochemical electrochemistry, adsorption and photodegradation, electrochemical oxygen reduction reaction, and fluorescence.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113355"},"PeriodicalIF":4.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142421410","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":"Boron vs. aluminum in ZSM-5 zeolites: Solid-state NMR, acidity, and C1/C2 reactant conversion","authors":"Michael Dyballa,&nbsp;Zheng Li ,&nbsp;Daniel Dittmann","doi":"10.1016/j.micromeso.2024.113353","DOIUrl":"10.1016/j.micromeso.2024.113353","url":null,"abstract":"<div><div>Three zeolite catalysts with comparable amounts of aluminum and/or boron ([Al]ZSM-5, [B,Al]ZSM-5, and [B]ZSM-5) are herein synthesized. Water (H₂O), ammonia (NH₃), acetonitrile-<em>d</em>₃ (ACN), and trimethylphosphine oxide (TMPO) are applied as probe molecules to investigate the acidity of the respective materials in combination with ¹¹B, ²⁷Al, and ²⁹Si MAS NMR spectroscopy. Ammonia is not protonated to ammonium on Si(OH)B groups and only LAS-bound ammonia persists desorption. Thus, ammonia gives a realistic, quantitative picture of the present acid sites. ACN interacts only with Si(OH)Al as desired. The strong base TMPO results in a misleading, not quantifiable picture. Subsequent hydration is unsuited to distinguish BAS and LAS densities. The samples were catalytically tested in the conversion of methanol, ethanol, and ethylene. [B]ZSM-5 is unreactive in hydrocarbon formation due to absence of BAS, instead LAS are present. The mixed [B,Al]ZSM-5 shows a decreased lifetime in MTO conversion compared to the [Al]ZSM-5, due to LAS presence. A sometimes reported superior reactivity of [B,Al]ZSM-5 catalysts is thus explained primarily by an optimized BAS density.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113353"},"PeriodicalIF":4.8,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142421421","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":"Crystallization process of LTA zeolite from alkoxides assisted by microwave heating","authors":"Kazuumi Ito ,&nbsp;Yuji Jinbo ,&nbsp;Wataru Fujiwara ,&nbsp;Takeshi Higuchi","doi":"10.1016/j.micromeso.2024.113343","DOIUrl":"10.1016/j.micromeso.2024.113343","url":null,"abstract":"<div><div>Microwave heating (MH) is a promising way for zeolite synthesis in terms of rapid and uniform reaction. However, detail process of the synthesis reaction and mechanism of its promotion by microwave are still under investigation. In the present study, LTA (Linde Type-A) zeolite was hydrothermally synthesized by 300 W of MH from hydrolyzed Al and Si alkoxides. The formation process of LTA was elucidated by nuclear magnetic resonance spectroscopy (²⁹Si NMR), small angle X-ray scattering (SAXS), X-ray diffraction (XRD), transmission electron microscopy (TEM), dynamic light scattering (DLS) and scanning electron microscopy (SEM). ²⁹Si NMR and SAXS analyses suggest that linear polycondensates of aluminosilicate in the precursor solution was immediately transformed into densely packed structure by MH. TEM observations reveals that crystalline phase with several nanometers was already formed in amorphous aluminosilicate nanoparticles prior to the MH while XRD shows that the amorphous phase had been transformed to LTA phase until 400 min of MH. It is basically consistent with the previous studies among zeolite synthesis assisted by both of conventional heating and MH. The aluminosilicate/LTA particle size was measured by DLS and SEM image as well as the yield was calculated from weight of the reaction products. The particle gradually grew up to 242 nm in diameter until 36 h while the yield sharply increased to nearly 100 % during 6.7 h and 12 h. In other words, all aluminosilicate in the solution once had polycondensed to form insoluble particle until 12 h followed by particle growth by dissolution-reprecipitation or agglomeration until 36 h.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113343"},"PeriodicalIF":4.8,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142421422","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":"Water in the micropores of CPO-27 metal-organic frameworks: A comprehensive study","authors":"Marvin Kloß,&nbsp;Christian Weinberger,&nbsp;Michael Tiemann","doi":"10.1016/j.micromeso.2024.113352","DOIUrl":"10.1016/j.micromeso.2024.113352","url":null,"abstract":"<div><div>The metal-organic framework CPO-27 exhibits free coordination sites (open metal sites) and can be prepared with a wide range of metals that influence its properties. It is therefore an intriguing structure to study sorption phenomena. We analyze the water resistance and sorption behavior of these frameworks, with particular attention to the sorption mechanism in detail and the structure of the confined water molecules. For this purpose, we use manometric water vapor sorption analysis and FTIR spectroscopy. The respective metal center orchestrates both the adsorption behavior and the arrangement of the water molecules in the micropores of the framework. The extent to which water molecules form hydrogen bonds (with each other and with framework oxygen atoms) plays a crucial role in the stability of the framework towards water. Water adsorption is governed by the coordination of water molecules to the open metal sites (except for CPO-27-Cu) and subsequent H-bonding. A stepwise adsorption of water is observed, with significant differences depending on the choice of metal.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113352"},"PeriodicalIF":4.8,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142356823","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":"A pyrene-based hydrogen-bonded framework with excimer induced ratiometric emission for discriminative luminescence detection of metal ions","authors":"Penglei Shen ,&nbsp;Hui Xu ,&nbsp;Tao Zhao ,&nbsp;Wei Zhang ,&nbsp;Gongxun Bai ,&nbsp;Thamraa Alshahrani ,&nbsp;Banglin Chen ,&nbsp;Junkuo Gao ,&nbsp;Shiqing Xu","doi":"10.1016/j.micromeso.2024.113348","DOIUrl":"10.1016/j.micromeso.2024.113348","url":null,"abstract":"<div><div>Discriminatory fluorescence detection of various metal ions is of significant importance in environmental and health-related applications. A luminescent hydrogen-bonded organic framework (HOF) material, PFC-1 was synthesized using 1,3,6,8-tetra(4-carboxylbenzene) pyrene (H₄TBAPy) as the organic building block. The fluorescence behavior of PFC-1 is influenced by the concentration of the suspension, demonstrating different emissions characteristic of monomer and excimer fluorescence, which are highly sensitive to the surrounding environment. This allows for the potential differentiation and sensing of different target analytes. PFC-1 showed discriminatory fluorescence sensing performance towards metal ions such as Al³⁺, Sc³⁺, Cr³⁺, and Cu²⁺, with changes in fluorescence intensity, emission peak shifts, and intensity ratio changes between monomer and excimer emissions. Furthermore, a smartphone-based detection strategy was proposed, leveraging color recognition capabilities of smartphones for onsite and real-time sensing. The work demonstrate that PFC-1 is a promising material for the development of portable, cost-effective fluorescent sensors for onsite and real-time detection of metal ions. The integration of PFC-1 with smartphone technology paves the way for practical applications in environmental monitoring, industrial processes, and healthcare diagnostics.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113348"},"PeriodicalIF":4.8,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142356825","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":"Rich active sites ZIF-8 base on imidazole-based deep eutectic solvents for rapid adsorption of acid fuchsin and competitive adsorption","authors":"Yiwen Li,&nbsp;Shikuan Xu,&nbsp;Yangyang Zhang,&nbsp;Rui Du,&nbsp;Rong Li,&nbsp;Yanjun Xing","doi":"10.1016/j.micromeso.2024.113351","DOIUrl":"10.1016/j.micromeso.2024.113351","url":null,"abstract":"<div><div>MimDES-ZIF-8 with rich active sites as positive charges and metal coordination sites were prepared based on imidazole based deep eutectic solvent (MimDES) using interface permeation method. 2-Methylimidazole (2-Mim) simultaneously acted as a hydrogen bond acceptor (HBA) in MimDES (hydrogen donner was 1,6-hexanediol) and an organic ligand in MimDES-ZIF-8, affecting the coordination of ZIF-8 during permeation. Four different zinc salt solutions (ZnCl₂, Zn(NO₃)₂·6H₂O, Zn(OAc)₂·2H₂O, ZnSO₄·7H₂O) were permeated into MimDES to obtain MimDES-ZIF-8 with different morphologies. All MimDES-ZIF-8 had higher Zn/N ration (&gt;0.25), specific surface area and surface positive charges. The dye adsorption results indicated that MimDES-ZIF-8 showed high adsorption efficiencies for acid fuchsin (all exceeded 97.75 % under pH 7.5) and a fast adsorption rate (exceeding 93 % in 5 min and reaching equilibrium in 60 min). Among MimDES-ZIF-8, the adsorption capacity of ZIF-8-C was 4845.3 mg/g. After five cycles of adsorption, the AF removal efficiency of ZIF-8-C remained over 93.23 %. Moreover, ZIF-8-C also had good adsorption capacity for anionic dyes CR, cationic dyes MB and BB. The adsorption process aligned well with both the Langmuir model and the pseudo-second-order kinetic model. Based on FTIR, XPS, and electrostatic potential calculation, the adsorption mechanism was elucidated.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113351"},"PeriodicalIF":4.8,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142326885","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":"Interfacial dynamics of Al3+ ions and water on hydrophilic adsorbents: A molecular dynamics study","authors":"Christopher Martínez López,&nbsp;Florianne Castillo-Borja","doi":"10.1016/j.micromeso.2024.113349","DOIUrl":"10.1016/j.micromeso.2024.113349","url":null,"abstract":"<div><div>The residues generated from the anodizing industry contain metallic ions like Al³⁺, and the presence of these pollutants in water bodies cause serious concern because of the ecological and human health risks. The adsorption of heavy metal ions is a widely used option due to it is an easy to implement, eco-friendly, and cost-effective process. This work reports the effect of different surfaces on the adsorption process of Al³⁺ ions to clarify the adsorption mechanism of the ions using molecular dynamics simulations. The models of three adsorbents: hydroxyapatite (HAP), an activated carbon (AC), and clinoptilolite (CLI) were computationally investigated to identify the most suitable adsorbent. The calculated adsorption isotherms allowed the evaluation of three different adsorbent materials for the removal of Al³⁺ ions from an aqueous solution. The findings were compared with experimental data of Al³⁺ adsorption onto bone char and a good qualitative similarity with experimental data was obtained for the HAP model. The results obtained by simulation as well as the experimental data fit satisfactorily to the Freundlich model, the fitting parameters show differences less than 3 % between the simulated and experimental data. For the three adsorbents, the simulated data fit better to the Freundlich isotherm adsorption model, suggesting heterogeneous adsorption on surfaces with variable adsorption capacity in each case. To study the adsorption mechanism, density profiles, RDFs, number of H-bonds, molecular minimum distances and intermolecular interactions were calculated. The efficiency of Al³⁺ ion adsorption is strongly influenced by the hydrophilic or amphiphilic nature of the adsorbent surface, as well as by the solvation structure of the ions in the solution. In each system, the solvation phenomenon occurs, although only the AC adsorbent exhibits it to a lesser extent compared to CLI and HAP surfaces. The CLI model had the highest adsorption capacity, due to its intense hydrophilic behavior, which leads to greater affinity and stability in the water molecules adsorbed on its surface and, therefore, allows a greater adsorption of Al³⁺ ions.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113349"},"PeriodicalIF":4.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142323613","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":"Fabrication of core-shell structural Y@VTMS-DVB composites with enhanced hydrophobicity for toluene capture under humid environment","authors":"Chang Lu,&nbsp;Xi Zhang,&nbsp;Pengfei Zhang,&nbsp;Lingling Ren,&nbsp;Nengjie Feng,&nbsp;Hui Wan,&nbsp;Guofeng Guan","doi":"10.1016/j.micromeso.2024.113350","DOIUrl":"10.1016/j.micromeso.2024.113350","url":null,"abstract":"<div><div>Zeolite Y serves as an effective adsorbent for VOCs capture due to its ordered porous structure, exceptional thermal stability, chemical resistance and fine-tune key properties. However, the hydrophilicity caused by the low SiO₂/Al₂O₃ ratio seriously limits its industrial application, especially in humid environments. In this work, a series of core-shell composites Y@VTMS-DVB_n were prepared through surface grafting and copolymerization. A variety of characterizations were utilized to study the structural and morphological changes of the prepared samples. The dynamic breakthrough adsorption experiment showed that the toluene uptake was significantly improved from 1.77 mg/g to 53.09 mg/g under 30 % relative humidity. Moreover, the core-shell composite exhibited excellent regeneration properties, the adsorption capacity remained 90 % under wet conditions after 6 cycles of regeneration. Adsorption kinetic analysis revealed that the adsorption behavior of toluene on the prepared adsorbents was primarily physical adsorption. These results show that the core-shell composite is a promising candidate for VOCs removal in industrial application.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"381 ","pages":"Article 113350"},"PeriodicalIF":4.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142323610","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}