Microporous and Mesoporous Materials最新文献

英文中文

Insight into the role of meso-Y zeolites in CsPMo/meso-Y composites on the selective oxidation of sulfides enhancement

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-16 DOI: 10.1016/j.micromeso.2025.113508

Chang Sun , Yutong Han , Yingzhen Wei , Zhong Zhang , Xiaohui Li , Guocheng Liu , Xiuli Wang

Polyoxometalates (POMs), renowned for their excellent catalytic activity, are widely used in oxidation reactions. Rational regulation of metal ion valence state of POMs is of great significance for the design and construction of highly active catalyst. In this work, we utilized mesoporous Y zeolite (meso-Y) as a host to load and disperse cesium phosphomolybdate (CsPMo) for selective oxidation of thioethers. The as-prepared CsPMo/meso-Y featured superior catalytic activity and recyclability. The electronic structures of the CsPMo/meso-Y were investigated by XPS and NMR spectra. The results indicated that embedding CsPMo into meso-Y caused electron transfer from CsPMo to meso-Y. Meanwhile, meso-Y could provide H⁺ due to its abundant Brønsted acid sites. The simultaneous appearance of electron and H⁺ facilitated the formation of Mo^V, resulting in a higher oxidation of thioethers activity for the CsPMo/meso-Y. Radical scavenger experiments and Raman analysis indicated that peroxo-metal species derived from CsPMo and oxidizing agent tert-butyl hydroperoxide (TBHP) were the real catalyst. Mo^V is more conducive to the formation of peroxo-metal species, causing the higher activity. This study provides a new insight into the role of meso-Y in CsPMo/meso-Y and a novel clue to regulate the valence states of metal ions of POMs to enhance catalytic performance of the polyoxometalate based catalysts.

{"title":"Insight into the role of meso-Y zeolites in CsPMo/meso-Y composites on the selective oxidation of sulfides enhancement","authors":"Chang Sun , Yutong Han , Yingzhen Wei , Zhong Zhang , Xiaohui Li , Guocheng Liu , Xiuli Wang","doi":"10.1016/j.micromeso.2025.113508","DOIUrl":"10.1016/j.micromeso.2025.113508","url":null,"abstract":"<div><div>Polyoxometalates (POMs), renowned for their excellent catalytic activity, are widely used in oxidation reactions. Rational regulation of metal ion valence state of POMs is of great significance for the design and construction of highly active catalyst. In this work, we utilized mesoporous Y zeolite (meso-Y) as a host to load and disperse cesium phosphomolybdate (CsPMo) for selective oxidation of thioethers. The as-prepared CsPMo/meso-Y featured superior catalytic activity and recyclability. The electronic structures of the CsPMo/meso-Y were investigated by XPS and NMR spectra. The results indicated that embedding CsPMo into meso-Y caused electron transfer from CsPMo to meso-Y. Meanwhile, meso-Y could provide H<sup>+</sup> due to its abundant Brønsted acid sites. The simultaneous appearance of electron and H<sup>+</sup> facilitated the formation of Mo<sup>V</sup>, resulting in a higher oxidation of thioethers activity for the CsPMo/meso-Y. Radical scavenger experiments and Raman analysis indicated that peroxo-metal species derived from CsPMo and oxidizing agent tert-butyl hydroperoxide (TBHP) were the real catalyst. Mo<sup>V</sup> is more conducive to the formation of peroxo-metal species, causing the higher activity. This study provides a new insight into the role of meso-Y in CsPMo/meso-Y and a novel clue to regulate the valence states of metal ions of POMs to enhance catalytic performance of the polyoxometalate based catalysts.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"387 ","pages":"Article 113508"},"PeriodicalIF":4.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143163598","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

Boosting the water absorption of CAU-10: The role of hydrochloric acid in regulating defect concentration

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-16 DOI: 10.1016/j.micromeso.2025.113510

Xiaoli Han , Ping Wu , Guodong Fu , Shiping Zhang , Li Wang , Min Xu , Xiulan Huai

CAU-10-H is a promising water adsorbent for adsorption heat transformation systems due to its excellent hydrothermal stability and favorable "S" type isothermal adsorption characteristic. However, its water uptake capacity is relatively low. In this work, the hydrochloric acid modulation defect structure of CAU-10 is rationally developed to get the CAU-10-HCl-2 sample, which possesses high water absorption capacity and outstanding cycle stability. The concentrations of metal atom defects and ligand defects in CAU-10-HCl-2 are 5.8 % and 3.0 %, respectively, which are 29 times and 0.375 times those of the CAU-10 sample without hydrochloric acid addition. This indicates that hydrochloric acid modulation facilitates the production of metal atom defects while suppressing the emergence of ligand defects. The specific surface area, micropore volume, and total pore volume of CAU-10-HCl-2 are 526.6 m²/g, 0.20 ml/g, and 0.23 ml/g, respectively, up 17 %, 25 %, and 10 % from CAU-10. At a relative pressure P/P₀ of 0.2, the water uptake of CAU-10-HCl-2 reaches up to 0.29 g/g, which is a 14 % increase compared to CAU-10. Compared to the initial hydration, the water uptake of CAU-10 decreases by 16 % by the 30th cycle, while that of CAU-10-HCl-2 lowers by only 2 %. These results demonstrate that hydrochloric acid modulation is an efficient strategy to improve the water absorption capacity and cyclic stability of CAU-10. This study provides quantitative analysis and synthesis instructions for designing defect structures in CAU-10 via hydrochloric acid modulation.

{"title":"Boosting the water absorption of CAU-10: The role of hydrochloric acid in regulating defect concentration","authors":"Xiaoli Han , Ping Wu , Guodong Fu , Shiping Zhang , Li Wang , Min Xu , Xiulan Huai","doi":"10.1016/j.micromeso.2025.113510","DOIUrl":"10.1016/j.micromeso.2025.113510","url":null,"abstract":"<div><div>CAU-10-H is a promising water adsorbent for adsorption heat transformation systems due to its excellent hydrothermal stability and favorable \"S\" type isothermal adsorption characteristic. However, its water uptake capacity is relatively low. In this work, the hydrochloric acid modulation defect structure of CAU-10 is rationally developed to get the CAU-10-HCl-2 sample, which possesses high water absorption capacity and outstanding cycle stability. The concentrations of metal atom defects and ligand defects in CAU-10-HCl-2 are 5.8 % and 3.0 %, respectively, which are 29 times and 0.375 times those of the CAU-10 sample without hydrochloric acid addition. This indicates that hydrochloric acid modulation facilitates the production of metal atom defects while suppressing the emergence of ligand defects. The specific surface area, micropore volume, and total pore volume of CAU-10-HCl-2 are 526.6 m<sup>2</sup>/g, 0.20 ml/g, and 0.23 ml/g, respectively, up 17 %, 25 %, and 10 % from CAU-10. At a relative pressure P/P<sub>0</sub> of 0.2, the water uptake of CAU-10-HCl-2 reaches up to 0.29 g/g, which is a 14 % increase compared to CAU-10. Compared to the initial hydration, the water uptake of CAU-10 decreases by 16 % by the 30th cycle, while that of CAU-10-HCl-2 lowers by only 2 %. These results demonstrate that hydrochloric acid modulation is an efficient strategy to improve the water absorption capacity and cyclic stability of CAU-10. This study provides quantitative analysis and synthesis instructions for designing defect structures in CAU-10 via hydrochloric acid modulation.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"387 ","pages":"Article 113510"},"PeriodicalIF":4.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143162782","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

Hydrocracking of polyethylene to high quality liquid fuels over bimetallic catalyst PdAg/HZSM-5

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-16 DOI: 10.1016/j.micromeso.2025.113512

Jie Liu , Xia Zhong , Li Gao , Ying Zhang , Ziru Wang , Mozaffar Shakeri , Xia Zhang , Bingsen Zhang

It is well known that the rapid accumulation of plastics poses a serious environmental pollution problem due to their difficulty in naturally decomposition. Hydrocracking provides an opportunity to convert plastics into value-added chemicals. Herein, the zeolite HZSM-5 supported metal bifunctional catalysts were synthesized for the hydrocracking of polyethylene to obtain high quality liquid hydrocarbon products. Benefiting from the strategy of bimetallic alloying, the second metal was designed to rationally regulate the structure of the active component within the catalyst in order to facilitate the conversion of polyolefin plastics into liquid hydrocarbons. It is found that the introduction of the second metal Ag could affect the electron density on Pd surface, which induced better dispersion of the metal particles. In addition, the metal-zeolite interactions as well as intermetallic interactions between these two metals can modulate the electronic state of Pd, thus improving the selectivity of the target products. The optimum Pd_0.5Ag_1.5/HZSM-5 catalyst was found to exhibit the best catalytic performance by tuning the Pd and Ag loading, with the liquid hydrocarbon yield of 69.18 %. The present work provides a reference for the design and synthesis of catalysts to improve the yield of high-value liquid fuels.

{"title":"Hydrocracking of polyethylene to high quality liquid fuels over bimetallic catalyst PdAg/HZSM-5","authors":"Jie Liu , Xia Zhong , Li Gao , Ying Zhang , Ziru Wang , Mozaffar Shakeri , Xia Zhang , Bingsen Zhang","doi":"10.1016/j.micromeso.2025.113512","DOIUrl":"10.1016/j.micromeso.2025.113512","url":null,"abstract":"<div><div>It is well known that the rapid accumulation of plastics poses a serious environmental pollution problem due to their difficulty in naturally decomposition. Hydrocracking provides an opportunity to convert plastics into value-added chemicals. Herein, the zeolite HZSM-5 supported metal bifunctional catalysts were synthesized for the hydrocracking of polyethylene to obtain high quality liquid hydrocarbon products. Benefiting from the strategy of bimetallic alloying, the second metal was designed to rationally regulate the structure of the active component within the catalyst in order to facilitate the conversion of polyolefin plastics into liquid hydrocarbons. It is found that the introduction of the second metal Ag could affect the electron density on Pd surface, which induced better dispersion of the metal particles. In addition, the metal-zeolite interactions as well as intermetallic interactions between these two metals can modulate the electronic state of Pd, thus improving the selectivity of the target products. The optimum Pd<sub>0.5</sub>Ag<sub>1.5</sub>/HZSM-5 catalyst was found to exhibit the best catalytic performance by tuning the Pd and Ag loading, with the liquid hydrocarbon yield of 69.18 %. The present work provides a reference for the design and synthesis of catalysts to improve the yield of high-value liquid fuels.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"387 ","pages":"Article 113512"},"PeriodicalIF":4.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143163597","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

Tunable acidity and porosity for optimizing liquid-phase catalytic efficiency utilizing hierarchical zeolite ZSM-5 single crystal reactor

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-15 DOI: 10.1016/j.micromeso.2025.113509

Zhan Liu , Jia-Min Lyu , Chun-Mu Guo , Zhi-Yi Hu , Ming-Hui Sun , Li-Hua Chen , Bao-Lian Su

Hierarchically porous zeolites, combining the intrinsic microporous catalytic properties and the enhanced meso-/macroporous access and transport, exhibit excellent performances in many highly efficient catalytic processes. The acidity and porosity are two key factors affecting the catalytic conversion, selectivity and lifetime. It is necessary to construct such hierarchically porous zeolite catalysts with adjustable acid active sites and pore properties in a wide range to meet the specific catalytic requirements. Herein, an ordered interconnected hierarchical ZSM-5 single crystal catalyst composed by zeolite sphere units stacking in face-centered cubic (FCC) arrangement has been used as the theoretical model to research the corresponding material properties on the enhancement of specific catalytic process. Specifically, the properties of acid sites and meso-/macropores can be accurately adjusted by facilely changing the SiO₂/Al₂O₃ molar ratio (100–1000) and the sphere unit size (180–580 nm), respectively. As a result, the benzyl alcohol liquid-phase catalytic ability markedly improved thanks to the optimized acidity and meso-/macropore size. The larger meso-/macropore size shows higher benzyl alcohol conversion, while the higher SiO₂/Al₂O₃ molar ratio exhibits higher alkylation product selectivity. This work illustrate that the targeted catalytic process can be effectively enhanced by adjusting the acidity and porosity within such ordered hierarchical ZSM-5 single crystal system.

{"title":"Tunable acidity and porosity for optimizing liquid-phase catalytic efficiency utilizing hierarchical zeolite ZSM-5 single crystal reactor","authors":"Zhan Liu , Jia-Min Lyu , Chun-Mu Guo , Zhi-Yi Hu , Ming-Hui Sun , Li-Hua Chen , Bao-Lian Su","doi":"10.1016/j.micromeso.2025.113509","DOIUrl":"10.1016/j.micromeso.2025.113509","url":null,"abstract":"<div><div>Hierarchically porous zeolites, combining the intrinsic microporous catalytic properties and the enhanced meso-/macroporous access and transport, exhibit excellent performances in many highly efficient catalytic processes. The acidity and porosity are two key factors affecting the catalytic conversion, selectivity and lifetime. It is necessary to construct such hierarchically porous zeolite catalysts with adjustable acid active sites and pore properties in a wide range to meet the specific catalytic requirements. Herein, an ordered interconnected hierarchical ZSM-5 single crystal catalyst composed by zeolite sphere units stacking in face-centered cubic (FCC) arrangement has been used as the theoretical model to research the corresponding material properties on the enhancement of specific catalytic process. Specifically, the properties of acid sites and meso-/macropores can be accurately adjusted by facilely changing the SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> molar ratio (100–1000) and the sphere unit size (180–580 nm), respectively. As a result, the benzyl alcohol liquid-phase catalytic ability markedly improved thanks to the optimized acidity and meso-/macropore size. The larger meso-/macropore size shows higher benzyl alcohol conversion, while the higher SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> molar ratio exhibits higher alkylation product selectivity. This work illustrate that the targeted catalytic process can be effectively enhanced by adjusting the acidity and porosity within such ordered hierarchical ZSM-5 single crystal system.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"387 ","pages":"Article 113509"},"PeriodicalIF":4.8,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143162778","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

Converting residues of fluid catalytic cracking catalysts into MOR/MFI with a full composite ratio via a crystal seed strategy

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-10 DOI: 10.1016/j.micromeso.2025.113492

Peng Lu , Yutong Che , Shuang Wu , Jinlei Zhang , Yiming Gao , Xiaosheng Wang , Yuxiang Liu

Considering the complex composition of fluid catalytic cracking catalyst residue (FCCR), it is a challenge to convert FCCR into MOR/MFI composite zeolites with a full composite ratio (i.e., MOR:MFI = 0: 100 %–100 %: 0). A crystal seed strategy is proposed to guide the crystallization phase and regulate properties such as porosity, morphology, acidity, and chemical coordination of MOR/MFI composite zeolites. In dehydration of glucose, MOR/MFI composite zeolite has a more excellent conversion of glucose and higher yield of 5-HMF than those of MOR zeolite. Based on the in-situ FTIR investigation, a higher concentration of fructose improve the dehydration to generate 5-HMF on MOR/MFI composite zeolites. Activation energy of dehydration of glucose decreases from 136.73 kJ/mol to 120.12 kJ/mol when using MOR/MFI composite zeolites. Proposed crystal seed strategy achieves the oriented conversion of FCCR to MOR/MFI composite zeolites with a desirable composition, which is also an important reference for other types of composite zeolites.

{"title":"Converting residues of fluid catalytic cracking catalysts into MOR/MFI with a full composite ratio via a crystal seed strategy","authors":"Peng Lu , Yutong Che , Shuang Wu , Jinlei Zhang , Yiming Gao , Xiaosheng Wang , Yuxiang Liu","doi":"10.1016/j.micromeso.2025.113492","DOIUrl":"10.1016/j.micromeso.2025.113492","url":null,"abstract":"<div><div>Considering the complex composition of fluid catalytic cracking catalyst residue (FCCR), it is a challenge to convert FCCR into MOR/MFI composite zeolites with a full composite ratio (i.e., MOR:MFI = 0: 100 %–100 %: 0). A crystal seed strategy is proposed to guide the crystallization phase and regulate properties such as porosity, morphology, acidity, and chemical coordination of MOR/MFI composite zeolites. In dehydration of glucose, MOR/MFI composite zeolite has a more excellent conversion of glucose and higher yield of 5-HMF than those of MOR zeolite. Based on the <em>in-situ</em> FTIR investigation, a higher concentration of fructose improve the dehydration to generate 5-HMF on MOR/MFI composite zeolites. Activation energy of dehydration of glucose decreases from 136.73 kJ/mol to 120.12 kJ/mol when using MOR/MFI composite zeolites. Proposed crystal seed strategy achieves the oriented conversion of FCCR to MOR/MFI composite zeolites with a desirable composition, which is also an important reference for other types of composite zeolites.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113492"},"PeriodicalIF":4.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155425","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

Stable and emissive covalent organic frameworks as highly sensitive and selective sensors for hydrazine

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-10 DOI: 10.1016/j.micromeso.2025.113506

Wanyi Zhao , Ce Xing , Yongfeng Zhi , He Li , Yuwei Zhang

Covalent organic frameworks (COFs) have attracted considerable interest owing to their lightweight properties, remarkable durability, and well-organized π-structures, positioning them as excellent candidates for emissive sensors. This research centers on the synthesis and characterization of two stable, emissive hydrazone-linked COFs (SEH-COFs) developed through solvothermal methods. The hydrazone linkages, together with the N-H single bond groups on the COF walls, are essential in reducing fluorescence quenching, which commonly occurs due to aggregation, thereby enhancing the emission activity of SEH-COFs. Furthermore, methoxy groups act as electron donors, delocalizing the electronic cloud from the vertex to the hydrazone linkage through p-π conjugation, which enhances the stability of SEH-COFs. The SEH-COFs obtain abundant interaction sites, primarily nitrogen and oxygen atoms, which facilitate efficient interactions with guest molecules. This feature contributes to the SEH-COFs' remarkable fluorescence quenching efficiency, reaching up to 82 %. Additionally, SEH-COFs exhibit high sensitivity and selectivity for hydrazine detection, with an exceptionally low detection limit of 0.78 nM in water, positioning them as one of the most effective fluorescent probes reported to date. This study emphasizes the importance of interaction sites in enhancing the performance of COF-based sensors and paves the way for developing high-performance emissive materials.

{"title":"Stable and emissive covalent organic frameworks as highly sensitive and selective sensors for hydrazine","authors":"Wanyi Zhao , Ce Xing , Yongfeng Zhi , He Li , Yuwei Zhang","doi":"10.1016/j.micromeso.2025.113506","DOIUrl":"10.1016/j.micromeso.2025.113506","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs) have attracted considerable interest owing to their lightweight properties, remarkable durability, and well-organized π-structures, positioning them as excellent candidates for emissive sensors. This research centers on the synthesis and characterization of two stable, emissive hydrazone-linked COFs (SEH-COFs) developed through solvothermal methods. The hydrazone linkages, together with the N-H single bond groups on the COF walls, are essential in reducing fluorescence quenching, which commonly occurs due to aggregation, thereby enhancing the emission activity of SEH-COFs. Furthermore, methoxy groups act as electron donors, delocalizing the electronic cloud from the vertex to the hydrazone linkage through p-π conjugation, which enhances the stability of SEH-COFs. The SEH-COFs obtain abundant interaction sites, primarily nitrogen and oxygen atoms, which facilitate efficient interactions with guest molecules. This feature contributes to the SEH-COFs' remarkable fluorescence quenching efficiency, reaching up to 82 %. Additionally, SEH-COFs exhibit high sensitivity and selectivity for hydrazine detection, with an exceptionally low detection limit of 0.78 nM in water, positioning them as one of the most effective fluorescent probes reported to date. This study emphasizes the importance of interaction sites in enhancing the performance of COF-based sensors and paves the way for developing high-performance emissive materials.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113506"},"PeriodicalIF":4.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155874","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

Elucidation of high activity and reaction mechanism for 1,2-dichloroethane catalytic oxidation over CoMnOx/HZSM-5 catalyst

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-10 DOI: 10.1016/j.micromeso.2025.113505

Peng Wang, Shilin Wu, Shuyun Ding, Ying Wang, Ningjie Fang, Yinghao Chu

The preparation of catalysts with excellent catalytic activity and stability in the catalytic oxidation of CVOCs by a simple and economical method with suitable support remained a challenge. For this reason, the MnCoO_x/HZ-x catalysts prepared by impregnation method with different Si/Al ratios of HZSM-5 as the support, and applied to the catalytic combustion of 1,2-dichloroethane (1,2-DCE). The results confirmed that the Si/Al ratio of the carrier affected the physicochemical properties of the surface active species, which improved the catalytic activity. The excellent catalytic activity (T₉₀ = 193 °C) and stability of MnCoO_x/HZ-25 were attributed to the abundance of Mn⁴⁺, Co²⁺, and surface adsorbed oxygen, the good redox capacity, and the suitable acidic strength stimulated by the lower Si/Al ratio of the carrier. In situ DRIFTS verified that at high temperatures and in the presence of oxygen, the production of vinyl alcohol or vinyl chloride species was not favored, and oxygenated intermediates such as carboxylates were mainly produced on MnCoO_x/HZ-25.

{"title":"Elucidation of high activity and reaction mechanism for 1,2-dichloroethane catalytic oxidation over CoMnOx/HZSM-5 catalyst","authors":"Peng Wang, Shilin Wu, Shuyun Ding, Ying Wang, Ningjie Fang, Yinghao Chu","doi":"10.1016/j.micromeso.2025.113505","DOIUrl":"10.1016/j.micromeso.2025.113505","url":null,"abstract":"<div><div>The preparation of catalysts with excellent catalytic activity and stability in the catalytic oxidation of CVOCs by a simple and economical method with suitable support remained a challenge. For this reason, the MnCoO<sub>x</sub>/HZ-x catalysts prepared by impregnation method with different Si/Al ratios of HZSM-5 as the support, and applied to the catalytic combustion of 1,2-dichloroethane (1,2-DCE). The results confirmed that the Si/Al ratio of the carrier affected the physicochemical properties of the surface active species, which improved the catalytic activity. The excellent catalytic activity (T<sub>90</sub> = 193 °C) and stability of MnCoO<sub>x</sub>/HZ-25 were attributed to the abundance of Mn<sup>4+</sup>, Co<sup>2+</sup>, and surface adsorbed oxygen, the good redox capacity, and the suitable acidic strength stimulated by the lower Si/Al ratio of the carrier. In situ DRIFTS verified that at high temperatures and in the presence of oxygen, the production of vinyl alcohol or vinyl chloride species was not favored, and oxygenated intermediates such as carboxylates were mainly produced on MnCoO<sub>x</sub>/HZ-25.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113505"},"PeriodicalIF":4.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155424","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

Effect of a mesoporous catalyst on total particulate matter generated during cigarette smoking

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-10 DOI: 10.1016/j.micromeso.2025.113487

Emilio Calabuig , Maribel Beltrán , Antonio Marcilla , Deseada Berenguer

During the smoking process, the volatiles and tars generated in a puff can condense or be adsorbed on the tobacco rod and the additive (if present), giving rise to secondary reactions. With aim of obtaining a better understanding of the effect of SBA-15 in reducing the amount of tars in the smoking process of tobacco SBA-15 mixtures, this work studies the effect of the SBA-15 additive on the pyrolysis of the total particulate matter (TPM) generated during the smoking process and condensed on the SBA-15. The studies developed by thermogravimetric analysis (TGA) and multi-shot pyrolyser (Py/GC/MS) show that the additive delays the decomposition of the TPM at higher temperatures. In addition, a lower amount of nicotine is observed, with greater reductions of the compounds generated during the decomposition at low temperatures and in an oxidizing atmosphere. These results explain the fact the smoking experiments show a significant reduction in the different families of compounds generated, both in the gaseous fraction and in the TPM, in presence of the additive, these reductions being generally higher than those observed when using other analysis techniques, where the secondary tar reactions of the adsorbed tars are not likely to occur.

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引用次数: 0

Copper nanoparticles confined in hollow silica spheres: Understanding the confinement effect and enhanced catalytic performance for the selective hydrogenation of dimethyl oxalate

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-10 DOI: 10.1016/j.micromeso.2025.113490

Bingwen Li , Junwei Liu , Yu Liu , Jinxian Zhao

Hollow silica spheres (HSS) supported Cu catalysts have been prepared by various methods and systematically characterized. The results indicated that impregnation method (IM) exhibits inferior dispersion of copper species. Compared to the deposition-precipitation (DP) and ammonia evaporation (AE) methods, the catalysts prepared by the one-pot (OP) method exhibit superior catalytic activity, evidenced by their MG yield being more than twice that achieved by the other two methods. This exceptional performance is attributed to the spatial confinement effect of HSS and the strong interaction between the Cu species and the silica support, which not only improves the dispersion of copper, reduces the size of Cu particles, but also enhances the amount of Cu⁺ species. Meanwhile, the positive correlation between the conversion of DMO and the amount of Cu⁺, and the formation of Cu⁺ species within the catalyst enhances the activation of the C-O and C=O bonds in DMO, leading to a marked enhancement in the catalytic performance during the hydrogenation.

{"title":"Copper nanoparticles confined in hollow silica spheres: Understanding the confinement effect and enhanced catalytic performance for the selective hydrogenation of dimethyl oxalate","authors":"Bingwen Li , Junwei Liu , Yu Liu , Jinxian Zhao","doi":"10.1016/j.micromeso.2025.113490","DOIUrl":"10.1016/j.micromeso.2025.113490","url":null,"abstract":"<div><div>Hollow silica spheres (HSS) supported Cu catalysts have been prepared by various methods and systematically characterized. The results indicated that impregnation method (IM) exhibits inferior dispersion of copper species. Compared to the deposition-precipitation (DP) and ammonia evaporation (AE) methods, the catalysts prepared by the one-pot (OP) method exhibit superior catalytic activity, evidenced by their MG yield being more than twice that achieved by the other two methods. This exceptional performance is attributed to the spatial confinement effect of HSS and the strong interaction between the Cu species and the silica support, which not only improves the dispersion of copper, reduces the size of Cu particles, but also enhances the amount of Cu<sup>+</sup> species. Meanwhile, the positive correlation between the conversion of DMO and the amount of Cu<sup>+</sup>, and the formation of Cu<sup>+</sup> species within the catalyst enhances the activation of the C-O and C=O bonds in DMO, leading to a marked enhancement in the catalytic performance during the hydrogenation.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113490"},"PeriodicalIF":4.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155970","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

Liquid metal interfacial engineering strategy to synthesize mesoporous carbon carbonized at mild temperature for the cycloaddition of CO2 with epoxides

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-01-09 DOI: 10.1016/j.micromeso.2025.113494

Pengyu Tang , Wenting Zhang , Duihai Tang , Shigang Xin , Zhen Zhao

In this study, we developed a liquid metal interfacial engineering strategy for the synthesis of mesoporous carbon through a liquid metal process. By using liquid Na/K alloy, a porous material with numerous C-Cl bonds was synthesized and carbon tetrachloride (CCl₄) as the precursor. Owing to the interaction between CCl₄ and the sodium–potassium alloy, both carbon and salts were produced in the system. The sodium chloride and potassium chloride formed during this process also acted as templating agents, which facilitated the formation of mesoporous structures. Furthermore, water washing effectively removed the salts. While this method previously demonstrated excellent surface activity for catalysts synthesized at room temperature, we modified the reaction temperature to further optimize performance, which resulted in mesoporous materials with larger pore structures and increased specific surface areas. Owing to the mild reaction temperature, this process not only increased the surface area and pore size of the product but also enhanced the carbon-chlorine bonds on its surface. In the cycloaddition of CO₂ with epoxides, the functionalized mesoporous carbon exhibited outstanding catalytic properties.

{"title":"Liquid metal interfacial engineering strategy to synthesize mesoporous carbon carbonized at mild temperature for the cycloaddition of CO2 with epoxides","authors":"Pengyu Tang , Wenting Zhang , Duihai Tang , Shigang Xin , Zhen Zhao","doi":"10.1016/j.micromeso.2025.113494","DOIUrl":"10.1016/j.micromeso.2025.113494","url":null,"abstract":"<div><div>In this study, we developed a liquid metal interfacial engineering strategy for the synthesis of mesoporous carbon through a liquid metal process. By using liquid Na/K alloy, a porous material with numerous C-Cl bonds was synthesized and carbon tetrachloride (CCl<sub>4</sub>) as the precursor. Owing to the interaction between CCl<sub>4</sub> and the sodium–potassium alloy, both carbon and salts were produced in the system. The sodium chloride and potassium chloride formed during this process also acted as templating agents, which facilitated the formation of mesoporous structures. Furthermore, water washing effectively removed the salts. While this method previously demonstrated excellent surface activity for catalysts synthesized at room temperature, we modified the reaction temperature to further optimize performance, which resulted in mesoporous materials with larger pore structures and increased specific surface areas. Owing to the mild reaction temperature, this process not only increased the surface area and pore size of the product but also enhanced the carbon-chlorine bonds on its surface. In the cycloaddition of CO<sub>2</sub> with epoxides, the functionalized mesoporous carbon exhibited outstanding catalytic properties.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"386 ","pages":"Article 113494"},"PeriodicalIF":4.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143155199","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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