Yang Zhou , Zhenzhu xia , Frank Peprah Addai , Jinping Chen , Chengxiang Feng , Zongjian Zhen , Juan Han , Feng Lin , Zhirong Wang , Yun Wang
{"title":"Hierarchically ordered truncated single crystal mesoporous ZIF-8 as a solid platform for lipase immobilization","authors":"Yang Zhou , Zhenzhu xia , Frank Peprah Addai , Jinping Chen , Chengxiang Feng , Zongjian Zhen , Juan Han , Feng Lin , Zhirong Wang , Yun Wang","doi":"10.1016/j.micromeso.2024.113430","DOIUrl":"10.1016/j.micromeso.2024.113430","url":null,"abstract":"<div><div>Most pristine metal organic frameworks (MOFs) are inherently microporous. To introduce desired porosity for easy enzyme infiltration and immobilization, polystyrene spheres was used as sacrificial template to design hierarchical ordered micro-mesoporous truncated single-crystalline ZIF-8 (SOM-ZIF-8). The surface area and pore diameter of the SOM-ZIF-8 were 821 m<sup>2</sup>/g and 7.09 nm which changed to 669 m<sup>2</sup>/g and 4.98 nm respectively, after lipase immobilization, suggesting the pores and surface of the SOM-ZIF-8 served as binding sites for the enzyme, and could reach a loading capacity of 134 mg/g after 24 h. The optimal conditions for achieving maximum lipase activity for free LipaseELP, ZIF-8@LipaseELP and SOM-ZIF-8@LipaseELP were pH 7.8 at 45 °C, and maintained 33.67 %, 45.6 % and 57.78 % residual activity after incubation at 80 °C for 2 h. The specific activity towards tributyrin and p-nitrophenyl acetate were observed to be SOM-ZIF-8@LipaseELP (0.25 and 45.85 U/mg) compared to ZIF-8@LipaseELP (0.211 and 43.62 U/mg) and LipaseELP (0.179 and 41.09 U/mg) respectively. The SOM-ZIF-8@LipaseELP could further be recovered and reused for 9 rounds while maintaining 73.8 % of its original activity. This study demonstrates that introducing mesoporous structures into ZIF-8 could improve its binding enzyme property for enhanced hydrolytic function.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"384 ","pages":"Article 113430"},"PeriodicalIF":4.8,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142697278","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}
Daniel D. Athayde , Giovana Magalhães dos Santos , Anna Carolina Britto de Faria , Camila de Lima Ribeiro , Carlos Martins Aiube , Daniel A.A. Ladislau , Edson Paulo da Silva , Luiz Fernando de Sousa Lima , Rodrigo Nunes de Souza , Saulo Lucas Pereira da Silva , Nelcy D.S. Mohallem , Alysson Martins Almeida Silva
{"title":"Investigation of the reaction time and hydrothermal synthesis route on the SSZ-13 zeolite particle crystallization and CO2 adsorption","authors":"Daniel D. Athayde , Giovana Magalhães dos Santos , Anna Carolina Britto de Faria , Camila de Lima Ribeiro , Carlos Martins Aiube , Daniel A.A. Ladislau , Edson Paulo da Silva , Luiz Fernando de Sousa Lima , Rodrigo Nunes de Souza , Saulo Lucas Pereira da Silva , Nelcy D.S. Mohallem , Alysson Martins Almeida Silva","doi":"10.1016/j.micromeso.2024.113428","DOIUrl":"10.1016/j.micromeso.2024.113428","url":null,"abstract":"<div><div>This study investigates the influence of synthesis time (1–4 days) and synthesis route for the fast production of SSZ-13 zeolites via the conventional hydrothermal method for CO<sub>2</sub> adsorption. Two synthesis routes were examined using different Si precursors: tetraethyorthosilicate (Route T) and silica (Route L). The samples were characterized by XRD, FTIR, SEM, <sup>29</sup>Si and <sup>27</sup>Al MAS-NMR, and gas sorption, the results were correlated to CO<sub>2</sub> adsorption kinetics. Route T produced fully crystalline SSZ-13 zeolite within 1 day with high yield, resulting in ultramicroporous materials through particle-mediate crystallization, transitioning from coarse spherical particles with high specific surface area (750 m<sup>2</sup> g<sup>−1</sup>) and the highest equilibrium CO<sub>2</sub> adsorption capacity of 81.08 mg g<sup>−1</sup>, to perfectly cubic structures for longer synthesis with decreased specific surface area (610 m<sup>2</sup> g<sup>−1</sup>) and porosity. A disorder-to-order transition for synthesis longer than 3 days, along with the elimination of the interspaces internal, significantly decreased CO<sub>2</sub> adsorption capacity (63.03 mg g<sup>−1</sup>). Meanwhile, SSZ-13 zeolites by Route L produced ultramicroporous crystalline particles only after 2 days, featuring intricate, layered structures formed by stacked sheets, indicating layer-by-layer mechanism. Longer synthesis times further increased particle complexity, reaching specific surface area of 858 m<sup>2</sup> g<sup>−1</sup> for the 4-day synthesis, along with improved CO<sub>2</sub> adsorption capacity. However, the CO<sub>2</sub> adsorption capacity for highly crystalline SSZ-13 samples obtained by Route L varied within 68.72–80.39 mg g<sup>−1</sup>, suggesting that structural properties also influenced CO<sub>2</sub> adsorption performance. These findings demonstrate that conventional hydrothermal synthesis can rapidly produce SSZ-13 adsorbents, allowing fine-tuning material properties and CO<sub>2</sub> adsorption capacity by selecting the appropriate synthesis route.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"384 ","pages":"Article 113428"},"PeriodicalIF":4.8,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142746543","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}
Boji Wang , Yao Zhang , Sarayute Chansai , Amal Nadri , Xiaoxia Ou , Qiang Zhang , Shaojun Xu , Yilai Jiao , Xiaolei Fan
{"title":"Selective catalytic reduction (SCR) of NOx with NH3 over the SSZ-13/ZSM-5 intergrowth zeolite","authors":"Boji Wang , Yao Zhang , Sarayute Chansai , Amal Nadri , Xiaoxia Ou , Qiang Zhang , Shaojun Xu , Yilai Jiao , Xiaolei Fan","doi":"10.1016/j.micromeso.2024.113429","DOIUrl":"10.1016/j.micromeso.2024.113429","url":null,"abstract":"<div><div>An intergrowth zeolite combining the SSZ-13 and ZSM-5 structure was synthesized using a dual-template method for application in selective catalytic reduction (SCR) of NO<sub>x</sub> with NH<sub>3</sub>. The intergrown structure was confirmed through detailed characterization. Compared to pure-phase zeolites, the intergrowth exhibited up to a 14 % enhancement in NO conversion at temperatures above 220 °C after hydrothermal aging (at 750 °C with 10 % H<sub>2</sub>O for 16 h). Comprehensive characterization revealed that intergrowth zeolite promoted the transformation of hydrothermally less stable Cu species (ZCuOH, located at 8 MR) to hydrothermally more stable Cu species (Z<sub>2</sub>Cu, located at 6 MR) during hydrothermal ageing. Additionally, copper leaching is hindered due to the well-preserved structural integrity of the intergrowth zeolite, with only a slight decrease in crystallinity (∼1.6 %). These findings suggest that intergrowth zeolites are promising candidates for mitigating NO<sub>x</sub> emissions in stationary sources under harsh hydrothermal conditions, such as that found in thermal power generation and steel manufacturing.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"384 ","pages":"Article 113429"},"PeriodicalIF":4.8,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142697276","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":"Facile coating Co/Ca-silicate on 13X for enhanced degradation of metronidazole via peroxymonosulfate activation: Catalytic performance and toxicity evolution","authors":"Qing Sun, Jiao Yan, Xiaofang Hu, Jiale Yu, Jian Zhang, Jiawei Sheng","doi":"10.1016/j.micromeso.2024.113424","DOIUrl":"10.1016/j.micromeso.2024.113424","url":null,"abstract":"<div><div>A facile urea-assisted hydrothermal method was developed for synthesizing Co(Ca)-silicate nanosheets@13X (CoCa-13X) as catalyst materials for peroxymonosulfate activation. Urea gradually dissolves 13X to form the silicate anion, and anchors Co<sup>2+</sup> ions to the surface of 13X, while introducing Ca<sup>2+</sup> ions to form in situ Co/Ca-silicates. The degradation efficiency and reusability of the compound catalyst for metronidazole (MNZ) were investigated. The results demonstrated that at an initial concentration of 25 mg/L, the CoCa-13X-PMS system exhibited excellent catalytic degradation performance towards MNZ, and the degradation rate reached 99.52 % within 5 min. Furthermore, the CoCa-13X-PMS system maintained high catalytic activity against various organic pollutants and even at high concentrations of pollutants (up to 30 mg/L). Free radical quenching experiments revealed simultaneous participation of SO<sub>4</sub><sup>•<strong>–</strong></sup> and <sup>1</sup>O<sub>2</sub> in the oxidation process simultaneously. Additionally, the degradation mechanism and pathway of MNZ were studied and proposed, along with evaluation of biotoxicity associated with its degradation intermediates. This method offers a novel strategy for synthesizing silica zeolite-based cobalt catalysts with exceptional PMS activity for removal of organic pollutants.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113424"},"PeriodicalIF":4.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706867","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":"Exploring statistical physics principles for superior Pefloxacin extraction from water via halloysite nanotubes: Stereographic and topographic evaluation","authors":"Amin Naifar , Kods Oueslati , Fatma Aouaini , Beriham Basha , Nadia Ayari , Abdelmottaleb Ben Lamine","doi":"10.1016/j.micromeso.2024.113427","DOIUrl":"10.1016/j.micromeso.2024.113427","url":null,"abstract":"<div><div>This novel research incorporates statistical physics methodologies to microscopically scrutinize and interpret the retention dynamics of Pefloxacin from aqueous solutions via Halloysite Nanotubes (HNTs) for water detoxification. Measurement points were matched under the scope of four distinct statistical isotherm frameworks: the single-energy monolayer, dual-energy monolayer, tri-energetic monolayer, and dual-energy bilayer. An error quantification approach, incorporating R<sup>2</sup>, reduced Chi-Square, RSS, and R<sup>2</sup><sub>adj</sub>, identified the dual-energy bilayer as the most suitable model. Rooted in the more realistic scenario, stereographic, energetic and thermodynamic parameters in addition to the pore size distribution (PSD) and adhesion energy distribution (AED) functions have been successfully developed and applied to examine the intricate details of the docking mechanisms. Stereographic examination unveiled that the linking cavities preferentially capture a majority of the attached species with n > 1 at specific temperatures indicating a specific-anchorage mechanism with substantial aggregation. Statistical thermodynamic exploration evidenced that the retention operation in this study is entropy-driven, and endothermic. Combining temperature and concentration impacts gives entropy a more complex behavior. Finally, the PSD and AED assessments revealed the mesoporous geometric size and energetic surface heterogeneity confirming the endothermic nature and physisorption-dominated mechanism (<25 kJ/mol) of the Pefloxacin/HNTs area-anchoring.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113427"},"PeriodicalIF":4.8,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706337","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}
Zaixing Yan, Wan Wang, Fangfang Zhao, Fei Liu, Tianxiang Zhao
{"title":"Direct synthesis of N-doped porous carbon materials from EDTA dipotassium salt for the rapid adsorption of hexavalent chromium from aqueous solutions","authors":"Zaixing Yan, Wan Wang, Fangfang Zhao, Fei Liu, Tianxiang Zhao","doi":"10.1016/j.micromeso.2024.113426","DOIUrl":"10.1016/j.micromeso.2024.113426","url":null,"abstract":"<div><div>The development of versatile, sustainable, and efficient N-doped porous carbon materials for the removal of trace contaminants has attracted considerable interest. Traditional methods for preparing porous carbon materials often involve the use of potent and hazardous activating agents such as KOH, H<sub>3</sub>PO<sub>4</sub>, and ZnCl<sub>2</sub>, which not only restrict the choice of production equipment but also pose environmental hazards. In this study, we introduce a self-activating method to synthesize N-doped porous carbon materials specifically designed for the removal of hexavalent chromium [Cr(VI)]. This approach involves the direct carbonization of EDTA dipotassium salt at different temperatures under a N<sub>2</sub> atmosphere without any activators. The influence of adsorbent dosages, pH, temperature, initial concentration of Cr(VI) ions, and competing ions on the adsorption behavior of Cr(VI) was systematically examined. The findings reveal that the optimal conditions for adsorption are a pH of 2 and an adsorbent dosage of 1.0 g L<sup>−1</sup>. Furthermore, Cr(VI) rapid adsorption onto N-doped porous carbon follows Freundlich isotherm and pseudo-second-order kinetic models. Notably, adsorbent KNC-700 exhibits an exceptional specific surface area of 2124.6 m<sup>2</sup> g<sup>−1</sup> and a well-defined pore structure. It shows maximum adsorption capacity for Cr(VI) of 270.3 mg g<sup>−1</sup> at 328 K with an equilibrium time of 20 min. Further mechanistic investigations suggest that efficient uptake of Cr(VI) primarily occurs through physico chemical adsorption involving electrostatic interactions and reduction reactions. This study provides novel insights into the preparation of porous carbon materials and their potential applications in addressing Cr(VI) pollution.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113426"},"PeriodicalIF":4.8,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706336","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}
Hang Xu , Ningxiang Lan , Yan Hu , Yuchun Xi , Jinzhi Hu , Chaowei Wen , Wanpeng Li , Chuanqiang Yin , Xiaomin Li , Lang Zhou
{"title":"Metal-organic framework/ 2D boron nitride nanosheets composite fillers in mixed matrix membranes for H2 /CO2 separation","authors":"Hang Xu , Ningxiang Lan , Yan Hu , Yuchun Xi , Jinzhi Hu , Chaowei Wen , Wanpeng Li , Chuanqiang Yin , Xiaomin Li , Lang Zhou","doi":"10.1016/j.micromeso.2024.113422","DOIUrl":"10.1016/j.micromeso.2024.113422","url":null,"abstract":"<div><div>Nanometer-thick two-dimensional (2D) materials are becoming ideal fillers for designing mixed matrix membranes (MMMs) with high gas permeability and selectivity due to their unique structures. ZIF-67@BNNS composite fillers were prepared by combining boron nitride nanosheets (BNNS), a thermally stable and chemically inert two-dimensional material, with the metal-organic framework ZIF-67. By incorporating these materials into polyetherimide (PEI), MMMs with efficient hydrogen (H<sub>2</sub>) separation performance have been developed. The -NH<sub>2</sub> groups on the BNNS surface provide a growth site for cobalt (Co) ions, facilitating the construction of a two-dimensional continuous channel by growing a ZIF-67 layer in situ on the BNNS surface. The inherent micropores of ZIF-67 create internal channels for gas transport within the composite packing, increasing gas permeability. The interlaced BNNS layer provides an external channel for gas transport, increasing resistance and contributing to improved gas selectivity. At a low loading of 1 wt%, the PEI/[email protected] MMMs exhibited a 199 % increase in H<sub>2</sub> permeability and 87 % improvement in H<sub>2</sub>/CO<sub>2</sub> selectivity compared to pure PEI membranes. In addition, these MMMs exhibit strong thermal stability and mechanical properties, making them promising for H<sub>2</sub> separation applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"384 ","pages":"Article 113422"},"PeriodicalIF":4.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142697277","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":"Mesoporous silica nanostructures embedding NIR active plasmonic nanoparticles: Harnessing antimicrobial agents delivery system for photo-assisted eradicating Gram-positive bacteria","authors":"Federica Rizzi , Elisabetta Fanizza , Mariangela Giancaspro , Nicoletta Depalo , Maria Lucia Curri , Blanca González , Montserrat Colilla , Isabel Izquierdo-Barba , María Vallet-Regí","doi":"10.1016/j.micromeso.2024.113414","DOIUrl":"10.1016/j.micromeso.2024.113414","url":null,"abstract":"<div><div>Implant-associated bone infection is increasingly emerging as a serious threat due to the high demand for orthopedic implants in our ageing society. Bacteria adhering to the surface of implants are highly resistant to conventional antibiotics and increasingly difficult to kill. In the quest for new antimicrobial strategies, multifunctional antimicrobial nanosystems offer new promise in the treatment of such infections. Herein, the development of mesoporous silica-coated plasmonic nanostructures for the delivery of antimicrobial drug for light-assisted therapy for bone infections is reported. Core@shell structures featuring Cu<sub>2-x</sub>S facet triangular nanoplates (NPL) core and a mesoporous silica shell (Cu<sub>2-x</sub>S@MSS) were synthesized. Further loading with antimicrobial molecules, such as levofloxacin (Levo) o rifampicin (Rif), allowed to synergistically combine the Cu<sub>2-x</sub>S NPL inherent antibacterial photoactivity with the pharmacological effects of the drug. The silica-based nanostructures, synthesized using a microemulsion approach, were thoroughly characterized, and their antibacterial activity explored in terms of inhibition of bacteria growth against <em>Staphylococcus aureus</em>. These results outline future applications of these nanoformulations for the management of bone implant-associated bacterial infections.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113414"},"PeriodicalIF":4.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706868","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":"Enhanced and rapid remediation of chlorpyrifos from aqueous phase by amine modified mesoporous silica SBA-15: A systematic investigation on sorption kinetics and mechanistic studies","authors":"Subhashree Mohanty, Sushanta Kumar Badamali","doi":"10.1016/j.micromeso.2024.113425","DOIUrl":"10.1016/j.micromeso.2024.113425","url":null,"abstract":"<div><div>Pesticides have become a necessary remedy of contemporary agricultural methods. However, the release of excess pesticides to the water bodies is a growing concern worldwide. Chlorpyrifos (CP), an organophosphate based pesticide used for nearly 50,000 tonnes per year globally, has significantly affected the ecosystem. Herein, we have reported that (3-Aminopropyl)triethoxysilane functionalized SBA-15 (ASBA-15) as an efficient adsorbent to remove CP from its aqueous solution to an extent of 1814 mg g<sup>−1</sup> within 20 min. The uptake behavior was studied in detail as a function of adsorbent dosage, contact time, and concentration levels of CP. The adsorption findings were well-fitted into the Langmuir isotherm model and pseudo-second-order kinetics. The estimated values of ΔH<sup>0</sup> and ΔS<sup>0</sup> revealed the exothermic and spontaneous nature of the process. The XRD reflections between 2 <span><math><mrow><mi>θ</mi></mrow></math></span> = 0.90–1.8<sup>o</sup>, surface area in the ranges of 781–435 m<sup>2</sup> g<sup>−1</sup> and pore diameters between 7.2 and 6.0nm indicated the mesoporous as well as stable structure for SBA-15 and ASBA-15 materials at different stages of studies. FT IR studies evidenced the presence of the ‒NH group at 1541 cm<sup>−1</sup> in ASBA-15. Thermogravimetric analysis results supported the grafting of the ‒NH group onto ASBA-15 as well as the efficient adsorption of CP. The appearance of characteristic vibration of CP at 1513 cm<sup>−1</sup> in CP@ASBA supported the entrapment of CP within ASBA-15. The adsorption and desorption of CP by ASBA-15 were accomplished for five cycles without significant mass loss, which demonstrated the reusability, stability and reversible nature of the material.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113425"},"PeriodicalIF":4.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142706866","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}
Eder Amayuelas , Sandeep Kumar Sharma , Jaideep Mor , Luis Bartolomé , Liam J.W. Johnson , Davide Caporale , Andrea Le Donne , Gianmarco Sigolo , Łukasz Scheller , Viviana Cristiglio , Pawel Zajdel , Simone Meloni , Yaroslav Grosu
{"title":"Effect of linker hybridization on the wetting of hydrophobic metal-organic frameworks","authors":"Eder Amayuelas , Sandeep Kumar Sharma , Jaideep Mor , Luis Bartolomé , Liam J.W. Johnson , Davide Caporale , Andrea Le Donne , Gianmarco Sigolo , Łukasz Scheller , Viviana Cristiglio , Pawel Zajdel , Simone Meloni , Yaroslav Grosu","doi":"10.1016/j.micromeso.2024.113423","DOIUrl":"10.1016/j.micromeso.2024.113423","url":null,"abstract":"<div><div>Wetting-dewetting of nanoporous materials is of key importance for a wide range of natural and technological cases, which include separation, chromatography, ionic channels. Heterogeneous lyophobic systems (HLS) consisting of a lyophobic nanoporous material and a non-wetting liquid are attractive for thermomechanical energy storage, conversion and dissipation under pressure/temperature variations. In recent years, metal-organic frameworks (MOFs) are entering many fields, including those mentioned above due to their wide structural diversity, structural flexibility and high tunability. In this work, we investigate the hitherto unexplored effects of forced wetting (intrusion-extrusion) of a hybrid mixed-linker ZIF-7-8 MOF (Zn-methylimidazole<sub>0.794</sub>–benzimidazole<sub>0.206</sub>) with water. Surprisingly, despite its structural similarity to ZIF-8, the hybrid ZIF-7-8 MOF demonstrates a non-hysteretic water intrusion-extrusion cycle that is in strong contrast to both ZIF-8 and ZIF-7 MOFs, which have pronounced intrusion-extrusion hysteresis. We used a combination of high-pressure intrusion-extrusion experiments, neutron diffraction structural analysis and atomistic simulations to put forward several hypotheses regarding the observed transformation from shock absorber/bumper behavior of ZIF-8 and ZIF-7 to molecular spring behavior of hybrid ZIF-7-8. These results open a new route for tuning the intrusion-extrusion (wetting-dewetting) hysteresis for numerous applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"383 ","pages":"Article 113423"},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658628","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}