Pub Date : 2025-01-08DOI: 10.1016/j.micromeso.2025.113502
Magdalena M. Lozinska , Elliott L. Bruce , Veselina M. Georgieva , Elizabeth M. Feverston , Shubhra J. Bhadra , Garret C. Lau , Timothy C. Golden , Erin M. Sorensen , Roger D. Whitley , Ronald I. Smith , Paul A. Wright , William J. Casteel (Jr)
The preparation of pure Ar from air requires removal of O2 from a crude Ar stream produced by cryogenic distillation. Whereas their similar boiling points make further separation by distillation expensive, the difference in their molecular sizes makes separation by flexible zeolites an attractive route to kinetic separation. Modifying the cation content of the flexible and cubic zeolite Rho enables precise tuning of a single window size for unprecedented kinetic separation of O2 from Ar. Li-Rho (unit cell Li9.8Al9.8Si38.2O96) is a very selective adsorbent due to its small pore size, but the highly distorted framework results in very slow O2 diffusion. By replacing some of the Li+ with H+, Cs+, or Zn2+, the window can be enlarged and in some cases the window cation occupancy reduced, increasing O2 diffusion rates whilst retaining high O2/Ar selectivity. The optimum unit cell composition among those examined was found to be Li6.2Zn1.8-Rho (O2/Ar selectivity = 813, D/r2(O2) = 0.37 s−1).
{"title":"Optimizing flexible zeolite Rho for unrivalled argon purification","authors":"Magdalena M. Lozinska , Elliott L. Bruce , Veselina M. Georgieva , Elizabeth M. Feverston , Shubhra J. Bhadra , Garret C. Lau , Timothy C. Golden , Erin M. Sorensen , Roger D. Whitley , Ronald I. Smith , Paul A. Wright , William J. Casteel (Jr)","doi":"10.1016/j.micromeso.2025.113502","DOIUrl":"10.1016/j.micromeso.2025.113502","url":null,"abstract":"<div><div>The preparation of pure Ar from air requires removal of O<sub>2</sub> from a crude Ar stream produced by cryogenic distillation. Whereas their similar boiling points make further separation by distillation expensive, the difference in their molecular sizes makes separation by flexible zeolites an attractive route to kinetic separation. Modifying the cation content of the flexible and cubic zeolite Rho enables precise tuning of a single window size for unprecedented kinetic separation of O<sub>2</sub> from Ar. Li-Rho (unit cell Li<sub>9.8</sub>Al<sub>9.8</sub>Si<sub>38.2</sub>O<sub>96</sub>) is a very selective adsorbent due to its small pore size, but the highly distorted framework results in very slow O<sub>2</sub> diffusion. By replacing some of the Li<sup>+</sup> with H<sup>+</sup>, Cs<sup>+</sup>, or Zn<sup>2+</sup>, the window can be enlarged and in some cases the window cation occupancy reduced, increasing O<sub>2</sub> diffusion rates whilst retaining high O<sub>2</sub>/Ar selectivity. The optimum unit cell composition among those examined was found to be Li<sub>6.2</sub>Zn<sub>1.8</sub>-Rho (O<sub>2</sub>/Ar selectivity = 813, <em>D/r</em><sup><em>2</em></sup>(O<sub>2</sub>) = 0.37 s<sup>−1</sup>).</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"387 ","pages":"Article 113502"},"PeriodicalIF":4.8,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143163599","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}
Pub Date : 2025-01-03DOI: 10.1016/j.micromeso.2024.113486
Huimin Zheng , Jiayue Niu , Yinan Liu , Shenfei Bai , Jing Ji , Shilin Tian , Zheyuan Tang
In gasoline deep desulfurization, the adsorption desulfurization technology encounters challenges due to the strong competitive interactions between aromatic molecules and thiophene compounds. This study investigates the competitive adsorption mechanism of benzene/thiophene mixtures in HY zeolites using molecular simulation at wide temperatures across full-loading spectra. The findings suggest that increasing the adsorption temperature can enhance thiophene selectivity by adjusting the interaction strength between the adsorbate and the zeolite framework. At loadings surpassing 40 molecules/UC, there is a fundamental shift in the competitive adsorption behavior of benzene and thiophene, impacting thiophene selectivity. The transition in competitive adsorption mechanisms is influenced by various factors, including the redistribution of adsorption sites, changes in adsorption energies, and the surface properties and pore structure of the zeolite framework. This research lays the theoretical groundwork for modifying the surface and mesoporous structure of zeolite frameworks to optimize adsorption behavior for improved thiophene selectivity in confined systems.
{"title":"Unlocking selective desulfurization: A molecular simulation dive into thiophene-benzene competition on HY zeolite","authors":"Huimin Zheng , Jiayue Niu , Yinan Liu , Shenfei Bai , Jing Ji , Shilin Tian , Zheyuan Tang","doi":"10.1016/j.micromeso.2024.113486","DOIUrl":"10.1016/j.micromeso.2024.113486","url":null,"abstract":"<div><div>In gasoline deep desulfurization, the adsorption desulfurization technology encounters challenges due to the strong competitive interactions between aromatic molecules and thiophene compounds. This study investigates the competitive adsorption mechanism of benzene/thiophene mixtures in HY zeolites using molecular simulation at wide temperatures across full-loading spectra. The findings suggest that increasing the adsorption temperature can enhance thiophene selectivity by adjusting the interaction strength between the adsorbate and the zeolite framework. At loadings surpassing 40 molecules/UC, there is a fundamental shift in the competitive adsorption behavior of benzene and thiophene, impacting thiophene selectivity. The transition in competitive adsorption mechanisms is influenced by various factors, including the redistribution of adsorption sites, changes in adsorption energies, and the surface properties and pore structure of the zeolite framework. This research lays the theoretical groundwork for modifying the surface and mesoporous structure of zeolite frameworks to optimize adsorption behavior for improved thiophene selectivity in confined systems.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113486"},"PeriodicalIF":4.8,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155876","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}
The regulations for emissions from internal combustion engine vehicles were becoming increasingly stringent, necessitating the development of cost-effective, high-performance purification materials. In this study, a HCs trap of kaolin-based ZSM-5 zeolite encapsulated ultra-low loading of Pt, with dual functions of adsorption and oxidation, was synthesized by a ligand-assisted hydrothermal method (Pt0.1@ZSM-5). The results of the corresponding adsorption-oxidation test demonstrated that the degradation efficiency of Pt0.1@ZSM-5 on propene reached 89.6 %, which could effectively reduce propene emission during cold-start period. More importantly, the degradation efficiency of Pt0.1@ZSM-5 on propene reached 67.9 % at the low temperature stage of 60 °C–160 °C. The primary reason for this was that the Pt0.1@ZSM-5 sample demonstrated exceptional catalytic activity with regard to propene oxidation, exhibiting a T90 of 192 °C. The confinement effect of zeolite resulted in the Pt0.1@ZSM-5 exhibiting a smaller nanoparticle size, an abundance of acidic sites, and a higher ratio of adsorbed oxygen. These properties contributed to the effective deep oxidation of propene. Furthermore, the degradation efficiency of propene was sustained at a high level (around 95 %) throughout the course of five adsorption-oxidation cycle tests. This study presented a novel approach for the functionalization and utilization of kaolin and provides guidance for its application in exhaust emissions during the cold-start period.
{"title":"Kaolin-derived ZSM-5 zeolite encapsulated with ultra-low loading of Pt catalysts for synergetic hydrocarbon adsorption/oxidation application","authors":"Langchuan Tian, Haotian Wang, Qijie Yi, Meijing Chen, Shengwei Tang, Wenxiang Tang","doi":"10.1016/j.micromeso.2025.113489","DOIUrl":"10.1016/j.micromeso.2025.113489","url":null,"abstract":"<div><div>The regulations for emissions from internal combustion engine vehicles were becoming increasingly stringent, necessitating the development of cost-effective, high-performance purification materials. In this study, a HCs trap of kaolin-based ZSM-5 zeolite encapsulated ultra-low loading of Pt, with dual functions of adsorption and oxidation, was synthesized by a ligand-assisted hydrothermal method (Pt<sub>0.1</sub>@ZSM-5). The results of the corresponding adsorption-oxidation test demonstrated that the degradation efficiency of Pt<sub>0.1</sub>@ZSM-5 on propene reached 89.6 %, which could effectively reduce propene emission during cold-start period. More importantly, the degradation efficiency of Pt<sub>0.1</sub>@ZSM-5 on propene reached 67.9 % at the low temperature stage of 60 °C–160 °C. The primary reason for this was that the Pt<sub>0.1</sub>@ZSM-5 sample demonstrated exceptional catalytic activity with regard to propene oxidation, exhibiting a T<sub>90</sub> of 192 °C. The confinement effect of zeolite resulted in the Pt<sub>0.1</sub>@ZSM-5 exhibiting a smaller nanoparticle size, an abundance of acidic sites, and a higher ratio of adsorbed oxygen. These properties contributed to the effective deep oxidation of propene. Furthermore, the degradation efficiency of propene was sustained at a high level (around 95 %) throughout the course of five adsorption-oxidation cycle tests. This study presented a novel approach for the functionalization and utilization of kaolin and provides guidance for its application in exhaust emissions during the cold-start period.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113489"},"PeriodicalIF":4.8,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155198","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}
Pub Date : 2025-01-03DOI: 10.1016/j.micromeso.2025.113488
Taekyung Ryu , Seung Hyeok Cha , Dong Won Hwang
In this study, we investigated the catalytic properties of the potassium-exchanged form of commercial and organic-free synthesized ZSM-5 zeolites with similar Si/Al and K/Al ratios (10–25 and 0.80–1.00, respectively) for the dehydration of biomass-derived methyl lactate to methyl acrylate under different reaction temperatures (340 and 360 °C) and reactant concentrations (35 and 64 wt%). It was found that organic-free synthesized K-ZSM-5 shows a higher methyl acrylate yield than commercially available K-ZSM-5, regardless of the reaction conditions studied. The comprehensive catalytic and characteristic findings from our study demonstrate that K+ ions, acting as active sites, are uniformly distributed within the 10-ring straight and sinusoidal channels of organic-free synthesized K-ZSM-5. This unique configuration imparts greater catalytic activity relative to commercially available K-ZSM-5 for the dehydration of methyl lactate to methyl acrylate with superior reusability even with identical zeolite topology and similar compositions.
{"title":"Catalytic dehydration of methyl lactate to methyl acrylate over potassium-exchanged organic-free ZSM-5 zeolites","authors":"Taekyung Ryu , Seung Hyeok Cha , Dong Won Hwang","doi":"10.1016/j.micromeso.2025.113488","DOIUrl":"10.1016/j.micromeso.2025.113488","url":null,"abstract":"<div><div>In this study, we investigated the catalytic properties of the potassium-exchanged form of commercial and organic-free synthesized ZSM-5 zeolites with similar Si/Al and K/Al ratios (10–25 and 0.80–1.00, respectively) for the dehydration of biomass-derived methyl lactate to methyl acrylate under different reaction temperatures (340 and 360 °C) and reactant concentrations (35 and 64 wt%). It was found that organic-free synthesized K-ZSM-5 shows a higher methyl acrylate yield than commercially available K-ZSM-5, regardless of the reaction conditions studied. The comprehensive catalytic and characteristic findings from our study demonstrate that K<sup>+</sup> ions, acting as active sites, are uniformly distributed within the 10-ring straight and sinusoidal channels of organic-free synthesized K-ZSM-5. This unique configuration imparts greater catalytic activity relative to commercially available K-ZSM-5 for the dehydration of methyl lactate to methyl acrylate with superior reusability even with identical zeolite topology and similar compositions.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113488"},"PeriodicalIF":4.8,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155423","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}
Pub Date : 2025-01-01DOI: 10.1016/j.micromeso.2024.113467
Alexander J. Hoffman , Mingrou Xie , Rafael Gómez-Bombarelli
Zeolite synthesis frequently relies on organic structure-directing agents (OSDAs), but the process of identifying the best OSDA to synthesize a given zeolite remains difficult. We use previously gathered binding energy data, in additional to the formation energies of the siliceous zeolite frameworks and approximate binding entropies of OSDAs to develop new descriptors to improve predictions based on known OSDA-zeolite pairs in the literature. Our earlier work used templating energy () to rank the most likely OSDA-zeolite pairs to be produced from synthesis. Using literature recall area-under-the-curve (AUC) as a performance metric, we find that computing energies associated with the net transformation that occurs during zeolite synthesis (the sum of the formation energy of the zeolite framework and the OSDA binding energy) provides a modest improvement over when predicting the zeolite phase that a given OSDA produces, from 67.5% average literature recall to 72.3%, but negligibly improves predictions for the best OSDA for a given zeolite framework, from 68.3% to 68.8%. We then use machine learning symbolic regression to develop a new descriptor, which we call , that slightly improves upon for predicting an OSDA for a given framework, with an average literature recall of 71.8%. While zeolite synthesis remains difficult to predict a priori, the approaches used in this work provide one option for improving these predictions.
{"title":"Learning descriptors to predict organic structure-directing agent applicability in zeolite synthesis","authors":"Alexander J. Hoffman , Mingrou Xie , Rafael Gómez-Bombarelli","doi":"10.1016/j.micromeso.2024.113467","DOIUrl":"10.1016/j.micromeso.2024.113467","url":null,"abstract":"<div><div>Zeolite synthesis frequently relies on organic structure-directing agents (OSDAs), but the process of identifying the best OSDA to synthesize a given zeolite remains difficult. We use previously gathered binding energy data, in additional to the formation energies of the siliceous zeolite frameworks and approximate binding entropies of OSDAs to develop new descriptors to improve predictions based on known OSDA-zeolite pairs in the literature. Our earlier work used templating energy (<span><math><msub><mrow><mi>E</mi></mrow><mrow><mi>i</mi><mi>j</mi><mo>,</mo><mi>T</mi></mrow></msub></math></span>) to rank the most likely OSDA-zeolite pairs to be produced from synthesis. Using literature recall area-under-the-curve (AUC) as a performance metric, we find that computing energies associated with the net transformation that occurs during zeolite synthesis (the sum of the formation energy of the zeolite framework and the OSDA binding energy) provides a modest improvement over <span><math><msub><mrow><mi>E</mi></mrow><mrow><mi>i</mi><mi>j</mi><mo>,</mo><mi>T</mi></mrow></msub></math></span> when predicting the zeolite phase that a given OSDA produces, from 67.5% average literature recall to 72.3%, but negligibly improves predictions for the best OSDA for a given zeolite framework, from 68.3% to 68.8%. We then use machine learning symbolic regression to develop a new descriptor, which we call <span><math><msub><mrow><mi>α</mi></mrow><mrow><mi>i</mi><mi>j</mi><mo>,</mo><mi>T</mi></mrow></msub></math></span>, that slightly improves upon <span><math><msub><mrow><mi>E</mi></mrow><mrow><mi>i</mi><mi>j</mi><mo>,</mo><mi>T</mi></mrow></msub></math></span> for predicting an OSDA for a given framework, with an average literature recall of 71.8%. While zeolite synthesis remains difficult to predict <em>a priori</em>, the approaches used in this work provide one option for improving these predictions.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113467"},"PeriodicalIF":4.8,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155236","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}
In this paper, the catalytic properties of novel granulated hierarchical (micro-meso-macroporous) zeolites H-Yh and H-ZSM-5h in the reaction of aniline and bio-1,2-propanediol are investigated. The influence of shape selectivity, textural and acid characteristics of zeolites on their activity and selectivity in the above reaction is shown. For the first time it was established that zeolite H-Yh was the most effective for obtaining 2-methyl-3-n-propyl-1H-indole 1 (yield 52 %), while 3,4-dimethyl-1-phenyl-1H-pyrrole 2 was obtained predominantly over zeolite H-ZSM-5h (yield 54 %). The conditions for compounds 1 and 2 with the maximum yield were determined. Possible pathways of the obtaining products are proposed, with consideration to the type, concentration and strength of acid sites, as well as the structural features of zeolites.
{"title":"Granulated hierarchical zeolites − novel pathways for utilizing bio-1,2-propanediol in the synthesis of practically important N-heterocycles","authors":"A.S. Artem'eva, N.G. Grigoreva, O.S. Travkina, S.V. Bubennov, D.V. Serebrennikov, B.I. Kutepov","doi":"10.1016/j.micromeso.2024.113478","DOIUrl":"10.1016/j.micromeso.2024.113478","url":null,"abstract":"<div><div>In this paper, the catalytic properties of novel granulated hierarchical (micro-meso-macroporous) zeolites H-Y<sub>h</sub> and H-ZSM-5<sub>h</sub> in the reaction of aniline and bio-1,2-propanediol are investigated. The influence of shape selectivity, textural and acid characteristics of zeolites on their activity and selectivity in the above reaction is shown. For the first time it was established that zeolite H-Y<sub>h</sub> was the most effective for obtaining 2-methyl-3-<em>n</em>-propyl-1H-indole <strong>1</strong> (yield 52 %), while 3,4-dimethyl-1-phenyl-1H-pyrrole <strong>2</strong> was obtained predominantly over zeolite H-ZSM-5<sub>h</sub> (yield 54 %). The conditions for compounds <strong>1</strong> and <strong>2</strong> with the maximum yield were determined. Possible pathways of the obtaining products are proposed, with consideration to the type, concentration and strength of acid sites, as well as the structural features of zeolites.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113478"},"PeriodicalIF":4.8,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155235","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}
Pub Date : 2024-12-28DOI: 10.1016/j.micromeso.2024.113485
Haijun Tan, Yi Yang , Na Qiu , Ruihan Tang, Ao Zhou, Jia Luo, Xiangfei Kong, Zhenguang Hu, Fuxin Zhong, Peipei Zhang
Developing porous organic materials for removing radiotoxic iodine from nuclear plant waste and heavy metal Fe3+ is significantly relevant to environmental remediation. To achieve reversible iodine adsorption, 1,6-dibromopyrene is used as the matrix, a unique nitrogen-rich porous organic polymer containing pyrene (PEMA) was tailor-made by introducing a triazine structure through a schiff base reaction. This polymer exhibits high affinity and adsorption capacity for iodine owing to its effective electron-rich adsorption sites, an extended π-conjugated structure and hierarchically porous structure. PEMA displayed remarkable adsorption capacities for saturated iodine vapor (3.19 g g−1) and iodine n-hexane solution (250.39 mg g−1). Furthermore, the fluorescence characteristic of PEMA has been employed for the selective detection of Fe3+ with high sensitivity with a low detection limit of 0.84 μM among a range of metal ions. Meanwhile, PEMA also demonstrates a good adsorption capacity for Fe3+, amounting to 48 mg g−1. These results suggest that PEMA possesses excellent iodine capture capabilities along with detection and adsorption capacities for Fe3+, making it a promising candidate for environmental remediation.
{"title":"Novel N-rich porous organic polymers for reversible iodine capture and selective detecting of Fe (III)","authors":"Haijun Tan, Yi Yang , Na Qiu , Ruihan Tang, Ao Zhou, Jia Luo, Xiangfei Kong, Zhenguang Hu, Fuxin Zhong, Peipei Zhang","doi":"10.1016/j.micromeso.2024.113485","DOIUrl":"10.1016/j.micromeso.2024.113485","url":null,"abstract":"<div><div>Developing porous organic materials for removing radiotoxic iodine from nuclear plant waste and heavy metal Fe<sup>3+</sup> is significantly relevant to environmental remediation. To achieve reversible iodine adsorption, 1,6-dibromopyrene is used as the matrix, a unique nitrogen-rich porous organic polymer containing pyrene (PEMA) was tailor-made by introducing a triazine structure through a schiff base reaction. This polymer exhibits high affinity and adsorption capacity for iodine owing to its effective electron-rich adsorption sites, an extended π-conjugated structure and hierarchically porous structure. PEMA displayed remarkable adsorption capacities for saturated iodine vapor (3.19 g g<sup>−1</sup>) and iodine n-hexane solution (250.39 mg g<sup>−1</sup>). Furthermore, the fluorescence characteristic of PEMA has been employed for the selective detection of Fe<sup>3+</sup> with high sensitivity with a low detection limit of 0.84 μM among a range of metal ions. Meanwhile, PEMA also demonstrates a good adsorption capacity for Fe<sup>3+</sup>, amounting to 48 mg g<sup>−1</sup>. These results suggest that PEMA possesses excellent iodine capture capabilities along with detection and adsorption capacities for Fe<sup>3+</sup>, making it a promising candidate for environmental remediation.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"385 ","pages":"Article 113485"},"PeriodicalIF":4.8,"publicationDate":"2024-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143137663","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}
Pub Date : 2024-12-28DOI: 10.1016/j.micromeso.2024.113484
Rui Gao, Mengxin Li, Yuanxue Li
This study aimed to synthesize drug-loaded hyper-crosslinked porous polymers (HCPs) under high-temperature, anhydrous, oxygen-free conditions through a Friedel–Crafts reaction. The resulting hyper-crosslinked porous polymers were characterized by infrared spectroscopy, nitrogen adsorption porosity measurements, thermo-gravimetric analysis, field-emission scanning electron microscopy, and powder X-ray diffraction for HCPs, and the electrochemical properties were investigated. The specific surface areas of the hyper-crosslinked porous polymers reached as high as 1079 m2g−1. We next investigated the use of one of the HCP samples as a drug delivery system and demonstrated its ability to release the model drug ibuprofen. Under selected synthesis conditions, the loading efficiency of the HCP with ibuprofen was 35 % (w/w). The release of the drug was also monitored, and 88 % of the loaded drug was released within 12 h. The resulting hyper-crosslinked porous polymer can be used as a matrix for the in vitro loading of ibuprofen.
{"title":"Synthesis of hyper-crosslinked porous polymers for drug release","authors":"Rui Gao, Mengxin Li, Yuanxue Li","doi":"10.1016/j.micromeso.2024.113484","DOIUrl":"10.1016/j.micromeso.2024.113484","url":null,"abstract":"<div><div>This study aimed to synthesize drug-loaded hyper-crosslinked porous polymers (HCPs) under high-temperature, anhydrous, oxygen-free conditions through a Friedel–Crafts reaction. The resulting hyper-crosslinked porous polymers were characterized by infrared spectroscopy, nitrogen adsorption porosity measurements, thermo-gravimetric analysis, field-emission scanning electron microscopy, and powder X-ray diffraction for HCPs, and the electrochemical properties were investigated. The specific surface areas of the hyper-crosslinked porous polymers reached as high as 1079 m<sup>2</sup>g<sup>−1</sup>. We next investigated the use of one of the HCP samples as a drug delivery system and demonstrated its ability to release the model drug ibuprofen. Under selected synthesis conditions, the loading efficiency of the HCP with ibuprofen was 35 % (w/w). The release of the drug was also monitored, and 88 % of the loaded drug was released within 12 h. The resulting hyper-crosslinked porous polymer can be used as a matrix for the in vitro loading of ibuprofen.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113484"},"PeriodicalIF":4.8,"publicationDate":"2024-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155237","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}
Pub Date : 2024-12-27DOI: 10.1016/j.micromeso.2024.113483
Sarah Haghjoo , Mohammad Kavand , Christian L. Lengauer , Hossein Kazemian , Mahmoud Roushani
This study explores the synthesis of a novel and efficient NaP1 zeolite from Austrian fly ash (AFA), composited with Fe3O4 nanoparticles (NPs) and lanthanum hydroxides [La(OH)3]. The composite's efficacy was tested for simultaneously adsorbing glyphosate (GLY), glufosinate (Glu), and aminomethylphosphonic acid (AMPA) from water solution. The inclusion of Fe3O4 NPs and La(OH)3 enhanced the nanoadsorbent's rapid and effective separation capabilities. Significantly, an innovative kinetic model, the Film-Pore-[Concentration-Dependent] Surface Diffusion Model (FPCDSD), was developed to analyze adsorption mechanisms, aligning with experimental results and accurately predicting adsorption processes in single and competitive scenarios. The model used detailed calculations to evaluate mass transfer resistances, employing parameters like rotation speed, adsorbent dosage, and initial concentrations to correlate adsorption data under various conditions. The study found that adsorption capacity retained 92 % effectiveness after 10 adsorption-desorption cycles, consistent with previous research. Results indicated that electrostatic interactions, herbicide affinity for La and Fe complexes, hydrogen bonding, and surface and pore diffusion likely drive adsorption mechanisms. Laboratory tests showed that Gly achieved the Maximum Residual Level (MRL) of 0.1 μg/L as per the European directive for drinking water with 99.95 % removal efficiency, suggesting that NaP1-Fe3O4-La(OH)3 is a highly effective option for water treatment.
{"title":"Enhanced herbicide removal using an innovative NaP1-Fe3O4-La(OH)3 zeolite: Advances in water treatment and experimental modeling","authors":"Sarah Haghjoo , Mohammad Kavand , Christian L. Lengauer , Hossein Kazemian , Mahmoud Roushani","doi":"10.1016/j.micromeso.2024.113483","DOIUrl":"10.1016/j.micromeso.2024.113483","url":null,"abstract":"<div><div>This study explores the synthesis of a novel and efficient NaP1 zeolite from Austrian fly ash (AFA), composited with Fe<sub>3</sub>O<sub>4</sub> nanoparticles (NPs) and lanthanum hydroxides [La(OH)<sub>3</sub>]. The composite's efficacy was tested for simultaneously adsorbing glyphosate (GLY), glufosinate (Glu), and aminomethylphosphonic acid (AMPA) from water solution. The inclusion of Fe<sub>3</sub>O<sub>4</sub> NPs and La(OH)<sub>3</sub> enhanced the nanoadsorbent's rapid and effective separation capabilities. Significantly, an innovative kinetic model, the Film-Pore-[Concentration-Dependent] Surface Diffusion Model (FPCDSD), was developed to analyze adsorption mechanisms, aligning with experimental results and accurately predicting adsorption processes in single and competitive scenarios. The model used detailed calculations to evaluate mass transfer resistances, employing parameters like rotation speed, adsorbent dosage, and initial concentrations to correlate adsorption data under various conditions. The study found that adsorption capacity retained 92 % effectiveness after 10 adsorption-desorption cycles, consistent with previous research. Results indicated that electrostatic interactions, herbicide affinity for La and Fe complexes, hydrogen bonding, and surface and pore diffusion likely drive adsorption mechanisms. Laboratory tests showed that Gly achieved the Maximum Residual Level (MRL) of 0.1 μg/L as per the European directive for drinking water with 99.95 % removal efficiency, suggesting that NaP1-Fe<sub>3</sub>O<sub>4</sub>-La(OH)<sub>3</sub> is a highly effective option for water treatment.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113483"},"PeriodicalIF":4.8,"publicationDate":"2024-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155234","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}
Pub Date : 2024-12-27DOI: 10.1016/j.micromeso.2024.113482
Lipeng Zhou , Haojie Zhang , Aiying Guo , Mengqing Wang , Zhihao Chen , Yunlai Su , Xiaomei Yang
Sn-Beta is a good Lewis acid catalyst. Typically, the organic template in as-made Sn-Beta was removed by calcination in air atmosphere at high temperature (≥500 °C). The fast combustion of organic template in air would lead that the actual temperature of sample is out of control, which will result in the partial disintegration of framework Sn species that are the active centers for catalytic reactions. In this work, ozonization at mild conditions (≤200 °C) was used to remove the organic template. It was found that the ozonization temperature greatly affected the template removal. The template removal efficiency reached 89 % at 120 °C for 3 h. The ozonized Sn-Beta has more framework Sn sites than Sn-Beta-C, for which the template was removed by traditional calcination route. However, the ozonized Sn-Beta showed slightly poor performance for conversion of glucose to methyl lactate (MLA) than Sn-Beta-C due to the presence of a few organic template. After the template residues were further removed by calcination of the ozonized Sn-Beta in air at 200–250 °C for 1 h, the catalytic performance of the ozonized Sn-Beta was significantly improved. Glucose conversion of 98.9 % with 48.7 % yield to MLA at 140 °C for 5 h was obtained over the ozonized Sn-Beta re-calcinated at 200 °C for 1 h.
{"title":"Effect of low-temperature ozonation-assisted detemplation on the properties and catalytic performance of Sn-Beta zeolite","authors":"Lipeng Zhou , Haojie Zhang , Aiying Guo , Mengqing Wang , Zhihao Chen , Yunlai Su , Xiaomei Yang","doi":"10.1016/j.micromeso.2024.113482","DOIUrl":"10.1016/j.micromeso.2024.113482","url":null,"abstract":"<div><div>Sn-Beta is a good Lewis acid catalyst. Typically, the organic template in as-made Sn-Beta was removed by calcination in air atmosphere at high temperature (≥500 °C). The fast combustion of organic template in air would lead that the actual temperature of sample is out of control, which will result in the partial disintegration of framework Sn species that are the active centers for catalytic reactions. In this work, ozonization at mild conditions (≤200 °C) was used to remove the organic template. It was found that the ozonization temperature greatly affected the template removal. The template removal efficiency reached 89 % at 120 °C for 3 h. The ozonized Sn-Beta has more framework Sn sites than Sn-Beta-C, for which the template was removed by traditional calcination route. However, the ozonized Sn-Beta showed slightly poor performance for conversion of glucose to methyl lactate (MLA) than Sn-Beta-C due to the presence of a few organic template. After the template residues were further removed by calcination of the ozonized Sn-Beta in air at 200–250 °C for 1 h, the catalytic performance of the ozonized Sn-Beta was significantly improved. Glucose conversion of 98.9 % with 48.7 % yield to MLA at 140 °C for 5 h was obtained over the ozonized Sn-Beta re-calcinated at 200 °C for 1 h.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"385 ","pages":"Article 113482"},"PeriodicalIF":4.8,"publicationDate":"2024-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143137667","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}
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