Microporous and Mesoporous Materials最新文献

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Simultaneous removal of tartrazine and erythrosine B using MnFe-layered double hydroxide nanoparticles modified PVDF polymer membrane

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-26 DOI: 10.1016/j.micromeso.2025.113569

Parsa Haroonian , Mehrorang Ghaedi , Hamedreza Javadian , Claudia Belviso , Mahboobeh Abbasi

Tartrazine (TZ) and erythrosine B (EB) dyes are extensively utilized as colorants in numerous commercial applications, including pharmaceuticals, textiles, and consumer products. However, their widespread use leads to the discharge of dye-containing wastewater, posing significant risks to aquatic ecosystems and human health. In this study, the simultaneous removal of these dyes was systematically investigated using MnFe-layered double hydroxides (LDHs)/PVDF as a composite membrane. A polyvinylidene fluoride (PVDF) polymer membrane was synthesized using the phase inversion method and subsequently modified with MnFe-LDH nanoparticles. The structural, morphological, and physicochemical properties of the prepared materials were characterized using XRD, BET, FT-IR, FE-SEM, EDS, and contact angle analyses. Critical operational parameters influencing the adsorption process, such as dye concentration, adsorption time, and adsorbent dosage, were systematically studied and optimized using response surface methodology (RSM) based on central composite design (CCD). In addition, the pH of the solution was optimized as a single independent variable. The impact of each parameter on the removal efficiency of the dyes was thoroughly analyzed. Optimization studies identified the following optimal conditions: Adsorption time = 15 min, the amount of adsorbent = 0.015 g, pH = 5, TZ = 16 mg/L, and EB = 13 mg/L. Under these conditions, removal efficiencies of 94.74 % and 92.13 % were achieved for TZ and EB dyes, respectively. The adsorption behavior was best described by the Langmuir isotherm model, indicating monolayer adsorption on a homogeneous surface. Kinetic evaluations revealed that the adsorption processes adhered closely to pseudo-first-order kinetic models. This study provides valuable insights into the development and application of MnFe-LDHs/PVDF composite membranes, highlighting their potential as effective materials for mitigating dye pollution in wastewater treatment systems.

{"title":"Simultaneous removal of tartrazine and erythrosine B using MnFe-layered double hydroxide nanoparticles modified PVDF polymer membrane","authors":"Parsa Haroonian , Mehrorang Ghaedi , Hamedreza Javadian , Claudia Belviso , Mahboobeh Abbasi","doi":"10.1016/j.micromeso.2025.113569","DOIUrl":"10.1016/j.micromeso.2025.113569","url":null,"abstract":"<div><div>Tartrazine (TZ) and erythrosine B (EB) dyes are extensively utilized as colorants in numerous commercial applications, including pharmaceuticals, textiles, and consumer products. However, their widespread use leads to the discharge of dye-containing wastewater, posing significant risks to aquatic ecosystems and human health. In this study, the simultaneous removal of these dyes was systematically investigated using MnFe-layered double hydroxides (LDHs)/PVDF as a composite membrane. A polyvinylidene fluoride (PVDF) polymer membrane was synthesized using the phase inversion method and subsequently modified with MnFe-LDH nanoparticles. The structural, morphological, and physicochemical properties of the prepared materials were characterized using XRD, BET, FT-IR, FE-SEM, EDS, and contact angle analyses. Critical operational parameters influencing the adsorption process, such as dye concentration, adsorption time, and adsorbent dosage, were systematically studied and optimized using response surface methodology (RSM) based on central composite design (CCD). In addition, the pH of the solution was optimized as a single independent variable. The impact of each parameter on the removal efficiency of the dyes was thoroughly analyzed. Optimization studies identified the following optimal conditions: Adsorption time = 15 min, the amount of adsorbent = 0.015 g, pH = 5, TZ = 16 mg/L, and EB = 13 mg/L. Under these conditions, removal efficiencies of 94.74 % and 92.13 % were achieved for TZ and EB dyes, respectively. The adsorption behavior was best described by the Langmuir isotherm model, indicating monolayer adsorption on a homogeneous surface. Kinetic evaluations revealed that the adsorption processes adhered closely to pseudo-first-order kinetic models. This study provides valuable insights into the development and application of MnFe-LDHs/PVDF composite membranes, highlighting their potential as effective materials for mitigating dye pollution in wastewater treatment systems.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"389 ","pages":"Article 113569"},"PeriodicalIF":4.8,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143526789","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

Bioinspired size separation of halloysite nanotubes by polydopamine-modified porous silica particles in matrix solid-phase dispersion fixed-bed column

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-26 DOI: 10.1016/j.micromeso.2025.113561

Zahra Kazemivalipour, Ali Nematollahzadeh, Taher Ataei-Germi, Zahra Vaseghi

Gradation of particles with a specific size range is crucial as it significantly impacts their properties and potential applications. In the present study, a mesoporous silica microsphere (MSMs) was synthesized and the surface chemistry was tuned by polydopamine (PDA) coating as a bioinspired polymer on the pore surfaces. The matrix solid-phase dispersion (MSPD) approach was exploited for the size classification of halloysite nanotubes (HNTs) of varying lengths. For this, the nanotubes were mixed with the as-prepared MSMs or with the PDA-modified silica microspheres (MSM/PDA) and packed in a column. The column was eluted with an aqueous solution of various pHs. The surface chemistry of MSM/PDA packings in synergy with their size exclusion nature led to the retention of the nanotubes of a specific size in the column. The results showed that the separation of HNTs by the MSM/PDA was carried out in far greater amounts (approximately 10-fold) compared with that of MSMs. The highest separation percentage of 32.87 % was achieved at pH 9 of the influent when MSM/PDA was used as packing. In addition, the size distribution analysis of HNTs in the first 10 mL of the effluent revealed that HNTs of average size of 442 nm with a lower polydispersity index value of 0.23 are achievable. Also, the various mathematical models were fitted to the experimental data for both MSMs-HNT and MSM/PDA-HNT packings. It was found that the second-order kinetic model well-suited the size separation of the nanotubes.

{"title":"Bioinspired size separation of halloysite nanotubes by polydopamine-modified porous silica particles in matrix solid-phase dispersion fixed-bed column","authors":"Zahra Kazemivalipour, Ali Nematollahzadeh, Taher Ataei-Germi, Zahra Vaseghi","doi":"10.1016/j.micromeso.2025.113561","DOIUrl":"10.1016/j.micromeso.2025.113561","url":null,"abstract":"<div><div>Gradation of particles with a specific size range is crucial as it significantly impacts their properties and potential applications. In the present study, a mesoporous silica microsphere (MSMs) was synthesized and the surface chemistry was tuned by polydopamine (PDA) coating as a bioinspired polymer on the pore surfaces. The matrix solid-phase dispersion (MSPD) approach was exploited for the size classification of halloysite nanotubes (HNTs) of varying lengths. For this, the nanotubes were mixed with the as-prepared MSMs or with the PDA-modified silica microspheres (MSM/PDA) and packed in a column. The column was eluted with an aqueous solution of various pHs. The surface chemistry of MSM/PDA packings in synergy with their size exclusion nature led to the retention of the nanotubes of a specific size in the column. The results showed that the separation of HNTs by the MSM/PDA was carried out in far greater amounts (approximately 10-fold) compared with that of MSMs. The highest separation percentage of 32.87 % was achieved at pH 9 of the influent when MSM/PDA was used as packing. In addition, the size distribution analysis of HNTs in the first 10 mL of the effluent revealed that HNTs of average size of 442 nm with a lower polydispersity index value of 0.23 are achievable. Also, the various mathematical models were fitted to the experimental data for both MSMs-HNT and MSM/PDA-HNT packings. It was found that the second-order kinetic model well-suited the size separation of the nanotubes.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"389 ","pages":"Article 113561"},"PeriodicalIF":4.8,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143520266","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

Highly controllable CO2 capture performance under varied humidity conditions by finely tuned metal and organic ligand compositions of DMOF adsorbents

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-24 DOI: 10.1016/j.micromeso.2025.113559

Xinyu Chen, Jinhai Leng, Fengying Ma, Jianqing Wu, Yi Jin, Miao Yu, Haomin Huang, Shanshan Shang, Daiqi Ye

Excessive CO₂ emissions significantly contribute to global warming, promoting the advancement of carbon capture and storage (CCS) technologies. Metal-organic frameworks (MOFs) are promising candidates for selective CO₂ adsorption; however, their effectiveness is often compromised in humid environments, such as flue gas streams. To overcome this limitation, this study synthesizes six isostructural DABCO-pillared MOFs (DMOFs) by finely tuning metal nodes (from Zn to Ni) and integrating methyl (-CH₃) functional groups on the organic ligand to enhance CO₂ adsorption performance, especially under humid conditions. Single gas adsorption isotherms reveal that the Ni-TM DMOF achieves the highest CO₂ adsorption capacity of 5.0 mmol g⁻¹ and maintains 100 % regenerability after five cycles. Binary CO₂/N₂ dynamic breakthrough experiments further demonstrate that the Ni-TM DMOF excels in both CO₂ uptake and CO₂/N₂ separation performance under both dry and humid conditions (80 % relative humidity). Mechanistic insights from in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations elucidate the molecular interactions between CO₂ and the DMOF structure, revealing that CO₂ adsorption predominantly occurs via physisorption, enhanced by C-H·O interaction from the -CH₃ groups. This work provides a strategic approach for enhancing the stability and efficiency of MOFs in industrial CO₂ sequestration applications.

{"title":"Highly controllable CO2 capture performance under varied humidity conditions by finely tuned metal and organic ligand compositions of DMOF adsorbents","authors":"Xinyu Chen, Jinhai Leng, Fengying Ma, Jianqing Wu, Yi Jin, Miao Yu, Haomin Huang, Shanshan Shang, Daiqi Ye","doi":"10.1016/j.micromeso.2025.113559","DOIUrl":"10.1016/j.micromeso.2025.113559","url":null,"abstract":"<div><div>Excessive CO<sub>2</sub> emissions significantly contribute to global warming, promoting the advancement of carbon capture and storage (CCS) technologies. Metal-organic frameworks (MOFs) are promising candidates for selective CO<sub>2</sub> adsorption; however, their effectiveness is often compromised in humid environments, such as flue gas streams. To overcome this limitation, this study synthesizes six isostructural DABCO-pillared MOFs (DMOFs) by finely tuning metal nodes (from Zn to Ni) and integrating methyl (-CH<sub>3</sub>) functional groups on the organic ligand to enhance CO<sub>2</sub> adsorption performance, especially under humid conditions. Single gas adsorption isotherms reveal that the Ni-TM DMOF achieves the highest CO<sub>2</sub> adsorption capacity of 5.0 mmol g<sup>−1</sup> and maintains 100 % regenerability after five cycles. Binary CO<sub>2</sub>/N<sub>2</sub> dynamic breakthrough experiments further demonstrate that the Ni-TM DMOF excels in both CO<sub>2</sub> uptake and CO<sub>2</sub>/N<sub>2</sub> separation performance under both dry and humid conditions (80 % relative humidity). Mechanistic insights from <em>in situ</em> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations elucidate the molecular interactions between CO<sub>2</sub> and the DMOF structure, revealing that CO<sub>2</sub> adsorption predominantly occurs <em>via</em> physisorption, enhanced by C-H·O interaction from the -CH<sub>3</sub> groups. This work provides a strategic approach for enhancing the stability and efficiency of MOFs in industrial CO<sub>2</sub> sequestration applications.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"389 ","pages":"Article 113559"},"PeriodicalIF":4.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143512206","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

Ti-grafting functionalization on alkali-etched nanozeolites to enhance their catalytic performance toward oxidation desulfurization of fuels

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-22 DOI: 10.1016/j.micromeso.2025.113556

Yichen Feng , Linghao Li , Jian Huang , Wei Wang , Bowen Lu , Siyu Yang , Haiwei Xu , Ying Shi , Zile Hua

Using silicalite-1 and TS-1 nanozeolites as precursors, a new combination process consisting of sequential alkali-etching and Ti-grafting treatment has been designed for preparation of hierarchically structured titanosilicate catalysts. The alkali-etching process creates abundant mesopores and Si-OH groups in the nanozeolite precursors, effectively increasing the titanium loadings and accelerating the mass transfer during the reactions. Benefiting from the developed micro/mesoporous structures, the adjustable Ti loadings and the intrinsic hydrophobicity of precursor nanozeolites, the resultant catalysts demonstrate superior performance toward the catalytic oxidation desulfurization (ODS) of fuels, i.e. in 3 h, the complete conversion of thiophene (Th), benzothiophene (BT) and dibenzothiophene (DBT) which are three typical refractory sulfur compounds with diverse reducibility and molecule sizes in fuels.

引用次数: 0

Corrigendum to “Manipulating pore structures of SSZ-13 zeolite membranes via hydrocracking activation for superior H2/CO2 separation” [Micropor. Mesopor. Mater. 387 (2025) 113518] 更正："通过加氢裂化活化操纵 SSZ-13 沸石膜的孔隙结构以实现卓越的 H2/CO2 分离" [Micropor. Mesopor. Mater. 387 (2025) 113518]

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-22 DOI: 10.1016/j.micromeso.2025.113551

Weibo Chen, Feng Ye, Shuanshi Fan, Yanhong Wang, Xuemei Lang, Zijian Zhang, Gang Li

引用次数: 0

Investigating the role of zeolite supports in Ni-based catalysts for CO2-methanation using in situ/operando XAS–GC-MS

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-22 DOI: 10.1016/j.micromeso.2025.113548

Waranya Obrom , Worapol Yingyuen , Tatchapol Nanmong , Krittanun Deekamwong , Pimrapus Tawachkultanadilok , Jatuporn Wittayakun , Sanchai Prayoonpokarach , Yingyot Poo-arporn , Karin Föttinger , Jean-Paul Desaulniers , Sirinuch Loiha

Nickel (Ni) is regarded as the most effective non-noble metal catalyst for CO₂ methanation. Its performance is strongly influenced by support material and Ni reducibility. This study investigates the impact of zeolite types (ANA, LTA, and ZSM-5) on the reducibility and catalytic performance of 5 wt% Ni catalysts, compared with SiO₂. Reducibility, measured via in situ X-ray absorption spectroscopy (XAS) from 100 to 450 °C, followed the order: 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/LTA > 5Ni/SiO₂. Catalytic testing in a fixed-bed flow reactor revealed the highest CO₂ conversion at 400 °C, following the order: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/SiO₂. Zeolite-supported catalysts achieved significantly higher CH₄ selectivity compared to 5Ni/SiO₂, with the trend: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA ≫ 5Ni/SiO₂. Comprehensive characterization using X-ray diffraction, N₂ adsorption-desorption, and X-ray photoelectron spectroscopy was conducted to analyze catalyst properties. The CO₂ methanation mechanism was deduced using data from in situ XAS-MS. These findings demonstrate that zeolite-supported Ni catalysts, particularly 5Ni/LTA, exhibit superior reducibility and catalytic performance, advancing the development of efficient materials for CO₂ conversion.

{"title":"Investigating the role of zeolite supports in Ni-based catalysts for CO2-methanation using in situ/operando XAS–GC-MS","authors":"Waranya Obrom , Worapol Yingyuen , Tatchapol Nanmong , Krittanun Deekamwong , Pimrapus Tawachkultanadilok , Jatuporn Wittayakun , Sanchai Prayoonpokarach , Yingyot Poo-arporn , Karin Föttinger , Jean-Paul Desaulniers , Sirinuch Loiha","doi":"10.1016/j.micromeso.2025.113548","DOIUrl":"10.1016/j.micromeso.2025.113548","url":null,"abstract":"<div><div>Nickel (Ni) is regarded as the most effective non-noble metal catalyst for CO<sub>2</sub> methanation. Its performance is strongly influenced by support material and Ni reducibility. This study investigates the impact of zeolite types (ANA, LTA, and ZSM-5) on the reducibility and catalytic performance of 5 wt% Ni catalysts, compared with SiO<sub>2</sub>. Reducibility, measured via in situ X-ray absorption spectroscopy (XAS) from 100 to 450 °C, followed the order: 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/LTA > 5Ni/SiO<sub>2</sub>. Catalytic testing in a fixed-bed flow reactor revealed the highest CO<sub>2</sub> conversion at 400 °C, following the order: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA > 5Ni/SiO<sub>2</sub>. Zeolite-supported catalysts achieved significantly higher CH<sub>4</sub> selectivity compared to 5Ni/SiO<sub>2</sub>, with the trend: 5Ni/LTA > 5Ni/ZSM-5 > 5Ni/ANA ≫ 5Ni/SiO<sub>2</sub>. Comprehensive characterization using X-ray diffraction, N<sub>2</sub> adsorption-desorption, and X-ray photoelectron spectroscopy was conducted to analyze catalyst properties. The CO<sub>2</sub> methanation mechanism was deduced using data from in situ XAS-MS. These findings demonstrate that zeolite-supported Ni catalysts, particularly 5Ni/LTA, exhibit superior reducibility and catalytic performance, advancing the development of efficient materials for CO<sub>2</sub> conversion.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"390 ","pages":"Article 113548"},"PeriodicalIF":4.8,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143579508","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

Mono- and bimetallic catalysts for the steam reforming of glycerol based on (Cox,Ni1-x)3Si2O5(OH)4 phyllosilicate nanoscrolls

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-21 DOI: 10.1016/j.micromeso.2025.113552

E.K. Khrapova, Sh. Omarov, A.A. Ivanova, D.A. Kirilenko, Yu. Kukushkina, A.A. Krasilin

Glycerol steam reforming is one of the potential method for hydrogen production is. Nanocomposites based on transition metal phyllosilicates may serve as promising candidates for the role of catalysts in this process. In the present work, Ni- Co-phyllosilicates with a pecoraite-like structure were studied. For the first time, a monometallic Co-catalyst (x = 1) and a bimetallic Ni-Co-catalyst (x = 0.4) were obtained and compared in a catalytic reaction of steam reforming of glycerol with a monometallic Ni-catalyst (x = 0) based on a nanotubular phyllosilicate with the general stoichiometric formula (Co_x,Ni_1-x)₃Si₂O₅(OH)₄. A series of physicochemical methods revealed differences in crystalline and porous structure, morphology of phyllosilicates, stability of porosity during reduction, and size and localization of metal nanoparticles. The catalysts were metal particles with dimensions of 9.6 ± 0.1 nm (x = 0), 11.2 ± 0.1 nm (x = 0.4), and 18.8 ± 0.4 nm (x = 1), dispersed in a phyllosilicate matrix as the support. For the sample with x = 0.4, the metal particles were a homogeneous NiCo alloy. This sample demonstrated a synergistic effect, which was manifested in an increase in glycerol conversion and hydrogen yield over time-on-stream at 600 °C as well as in higher stability and a lower tendency to coking in compared to monometallic samples. The identified features of the studied systems (increase in the homogeneity of the NiCo alloy during the test, oxidation and blocking of Co nanoparticles inside the phyllosilicate channels) made it possible to explain the observed differences in the catalytic behavior in the steam conversion of glycerol.

甘油蒸汽转化是一种潜在的制氢方法。基于过渡金属绿硅酸盐的纳米复合材料有可能成为该过程中的催化剂。在本研究中，研究人员研究了具有白云石状结构的镍-钴-方硅酸盐。在甘油蒸汽转化的催化反应中，首次获得了单金属 Co 催化剂（x = 1）和双金属 Ni-Co 催化剂（x = 0.4），并与基于纳米管状辉绿硅酸盐的单金属 Ni 催化剂（x = 0）进行了比较，后者的化学计量学通式为 (Cox,Ni1-x)3Si2O5(OH)4 。一系列物理化学方法揭示了结晶和多孔结构、植硅酸盐的形态、还原过程中孔隙率的稳定性以及金属纳米颗粒的尺寸和定位等方面的差异。催化剂的金属颗粒尺寸分别为 9.6 ± 0.1 nm（x = 0）、11.2 ± 0.1 nm（x = 0.4）和 18.8 ± 0.4 nm（x = 1），分散在作为支撑物的植硅酸盐基质中。在 x = 0.4 的样品中，金属颗粒是均匀的镍钴合金。与单金属样品相比，该样品具有协同效应，表现为在 600 °C 下，随着时间的推移，甘油转化率和氢气产量增加，稳定性提高，结焦倾向降低。所研究体系的特征（镍钴合金在试验过程中的均匀性增加、钴纳米颗粒在植硅体通道内的氧化和阻塞）可以解释在蒸汽转化甘油过程中观察到的催化行为差异。

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引用次数: 0

A novel Z-scheme Ag/AgBr/Bi4O5Br2 heterojunction with rich oxygen vacancy for enhanced photocatalytic degradation of formaldehyde

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-20 DOI: 10.1016/j.micromeso.2025.113555

Qinghai Zhang , Weiweng Wang , Yunlong Qu , Mengqi Bian , Rui Liu , Guanghui Chen , Chaojie Li , Jihai Duan

Fabrication of a plasma-based Z-scheme heterojunction can significantly accelerate the charge separation and broaden the light response range. Herein, a series of Ag/AgBr/Bi₄O₅Br₂-x% (abbr. A/AB/BOB-x%; x = 5, 10, 30 and 50) Z-scheme heterojunctions containing rich oxygen vacancies (Ovs) were successfully synthesized via the alcoholysis method, followed by ion-exchange and photoreduction method to enhance photocatalytic formaldehyde degradation. The formaldehyde degradation efficiency of A/AB/BOB-10 % composite reached 94.3 % at 3 h of light irradiation, which was 1.6, 1.2 and 2.3 times higher than that of BiOBr (60.1 %), BOB (78.3 %) and Ag/AgBr (41.2 %), respectively. The enhanced photodegradation activity was ascribed to the synergistic effects arising from the formation of Z-scheme heterojunction, the surface plasmon resonance (SPR) effect induced by Ag nanoparticles (Ag NPs) and the rich oxygen vacancies. Moreover, the cycle experiments demonstrated that A/AB/BOB-10 % composite had favorable stability and repeatability, achieving a degradation efficiency of 81.2 %. The electron spin resonance (ESR) and radical capturing tests demonstrated that the active species involved in photocatalytic degradation of formaldehyde include h⁺, ·OH and ·O₂⁻, with h⁺ playing a predominant role. Additionally, ion chromatography revealed that formic acid (HCOOH) was an intermediate during the removal process of formaldehyde. Finally, the Z-scheme charge transfer mechanism bridged by Ag NPs for the photocatalytic degradation of formaldehyde was proposed based on the ESR tests and an analysis of energy band structure. The current study presents a promising approach for the fabrication of high-efficiency plasma-based Z-scheme heterojunction photocatalysts for formaldehyde degradation.

{"title":"A novel Z-scheme Ag/AgBr/Bi4O5Br2 heterojunction with rich oxygen vacancy for enhanced photocatalytic degradation of formaldehyde","authors":"Qinghai Zhang , Weiweng Wang , Yunlong Qu , Mengqi Bian , Rui Liu , Guanghui Chen , Chaojie Li , Jihai Duan","doi":"10.1016/j.micromeso.2025.113555","DOIUrl":"10.1016/j.micromeso.2025.113555","url":null,"abstract":"<div><div>Fabrication of a plasma-based Z-scheme heterojunction can significantly accelerate the charge separation and broaden the light response range. Herein, a series of Ag/AgBr/Bi<sub>4</sub>O<sub>5</sub>Br<sub>2</sub>-<em>x</em>% (<em>abbr</em>. A/AB/BOB-<em>x</em>%; <em>x</em> = 5, 10, 30 and 50) Z-scheme heterojunctions containing rich oxygen vacancies (Ovs) were successfully synthesized via the alcoholysis method, followed by ion-exchange and photoreduction method to enhance photocatalytic formaldehyde degradation. The formaldehyde degradation efficiency of A/AB/BOB-10 % composite reached 94.3 % at 3 h of light irradiation, which was 1.6, 1.2 and 2.3 times higher than that of BiOBr (60.1 %), BOB (78.3 %) and Ag/AgBr (41.2 %), respectively. The enhanced photodegradation activity was ascribed to the synergistic effects arising from the formation of Z-scheme heterojunction, the surface plasmon resonance (SPR) effect induced by Ag nanoparticles (Ag NPs) and the rich oxygen vacancies. Moreover, the cycle experiments demonstrated that A/AB/BOB-10 % composite had favorable stability and repeatability, achieving a degradation efficiency of 81.2 %. The electron spin resonance (ESR) and radical capturing tests demonstrated that the active species involved in photocatalytic degradation of formaldehyde include h<sup>+</sup>, ·OH and ·O<sub>2</sub><sup>−</sup>, with h<sup>+</sup> playing a predominant role. Additionally, ion chromatography revealed that formic acid (HCOOH) was an intermediate during the removal process of formaldehyde. Finally, the Z-scheme charge transfer mechanism bridged by Ag NPs for the photocatalytic degradation of formaldehyde was proposed based on the ESR tests and an analysis of energy band structure. The current study presents a promising approach for the fabrication of high-efficiency plasma-based Z-scheme heterojunction photocatalysts for formaldehyde degradation.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"389 ","pages":"Article 113555"},"PeriodicalIF":4.8,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474555","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

Amorphousness matters: Its role on nonpolar gas diffusion at the nanoscale

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-19 DOI: 10.1016/j.micromeso.2025.113540

Solana M. Di Pino, Oscar Churio, Ezequiel de la Llave, Verónica M. Sánchez

Amorphous carbon materials (ACM) produced using biomass waste feedstocks, offers an affordable, large-scale, and environmentally friendly production method. Their inherent porosity critically impacts gas diffusion and various applications, including gas separation, purification, and catalysis. This work determines, through molecular dynamics simulations, the effect of amorphicity on the diffusion of pure oxygen and methane, their 50% mixture and a 50% mixture of methane and carbon dioxide. For pure systems, we compare ACM with pores of similar size and regular shapes, such as slit pores and carbon nanotubes, with and without surface roughness. From the analysis of diffusion trajectories we find that molecular mobility decreases as the surface structural constrictions increase, configuring a more intricate molecular path for the gas to surface-diffuse. Specifically, constrictions imposed by the carbon surface structure increase in the next order: smooth surfaces, rough CNTs and ACMs. For ACM with a pore diameter of 1.5 nm, gas diffusion decreased by up to 95%. Notably, oxygen was trapped in surface defects (“pockets”) for both pure oxygen and its mixture with methane. The effects of pressure and temperature on the dynamic behavior of mixtures were also explored. For the 50% mixture of carbon dioxide and methane, we observed that in ACM with the smallest pore size, the relative diffusion is reduced by around 50% compared to bulk. Our findings suggest that amorphous materials could be preferred for devices that require high selectivity between gas mixtures due to their specific porous structure.

{"title":"Amorphousness matters: Its role on nonpolar gas diffusion at the nanoscale","authors":"Solana M. Di Pino, Oscar Churio, Ezequiel de la Llave, Verónica M. Sánchez","doi":"10.1016/j.micromeso.2025.113540","DOIUrl":"10.1016/j.micromeso.2025.113540","url":null,"abstract":"<div><div>Amorphous carbon materials (ACM) produced using biomass waste feedstocks, offers an affordable, large-scale, and environmentally friendly production method. Their inherent porosity critically impacts gas diffusion and various applications, including gas separation, purification, and catalysis. This work determines, through molecular dynamics simulations, the effect of amorphicity on the diffusion of pure oxygen and methane, their 50% mixture and a 50% mixture of methane and carbon dioxide. For pure systems, we compare ACM with pores of similar size and regular shapes, such as slit pores and carbon nanotubes, with and without surface roughness. From the analysis of diffusion trajectories we find that molecular mobility decreases as the surface structural constrictions increase, configuring a more intricate molecular path for the gas to surface-diffuse. Specifically, constrictions imposed by the carbon surface structure increase in the next order: smooth surfaces, rough CNTs and ACMs. For ACM with a pore diameter of 1.5 nm, gas diffusion decreased by up to 95%. Notably, oxygen was trapped in surface defects (“pockets”) for both pure oxygen and its mixture with methane. The effects of pressure and temperature on the dynamic behavior of mixtures were also explored. For the 50% mixture of carbon dioxide and methane, we observed that in ACM with the smallest pore size, the relative diffusion is reduced by around 50% compared to bulk. Our findings suggest that amorphous materials could be preferred for devices that require high selectivity between gas mixtures due to their specific porous structure.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"388 ","pages":"Article 113540"},"PeriodicalIF":4.8,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Adsorption behavior of low-concentration nitrous oxide on natural mordenite zeolite

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-17 DOI: 10.1016/j.micromeso.2025.113550

Saeko Yamaguchi , Peidong Hu , Hanlong Ya , Peipei Xiao , Ayako Nakata , Tsuyoshi Miyazaki , Yoshitada Morikawa , Junko N. Kondo , Kotaro Tange , Kenichi Tonokura , Masanori Takemoto , Yasuo Yonezawa , Toshiyuki Yokoi , Kenta Iyoki , Tatsuya Okubo , Toru Wakihara

Nitrous oxide (N₂O), the third most important greenhouse gas, is discharged from various anthropogenic sources and causes severe environmental problems. Herein, the natural mordenite zeolite is demonstrated to be an effective adsorbent to capture low-concentration N₂O (below 30 ppm). An adsorption capacity of 0.076 mmol g⁻¹ can be achieved at −7 °C with 1 ppm N₂O in the dynamic adsorption test, 6.3 times as high as that at 25 °C. The density functional theory calculations reveal that the Ca-exchanged MOR-type zeolite has stronger interactions with N₂O compared with the Na-exchanged one. However, as evidenced by the isosteric adsorption enthalpy analysis and the Fourier transform infrared spectroscopy, the natural mordenite zeolite with both Na⁺ and Ca²⁺, as well as the synthesized analogue, demonstrates stronger and distinctive interactions with trace N₂O in comparison to the MOR-type zeolites with single kind of extra-framework cation. These results provide experimental and theoretical foundations for the establishment of efficient N₂O removal system using well designed zeolite-based adsorbents under proper operating conditions.

{"title":"Adsorption behavior of low-concentration nitrous oxide on natural mordenite zeolite","authors":"Saeko Yamaguchi , Peidong Hu , Hanlong Ya , Peipei Xiao , Ayako Nakata , Tsuyoshi Miyazaki , Yoshitada Morikawa , Junko N. Kondo , Kotaro Tange , Kenichi Tonokura , Masanori Takemoto , Yasuo Yonezawa , Toshiyuki Yokoi , Kenta Iyoki , Tatsuya Okubo , Toru Wakihara","doi":"10.1016/j.micromeso.2025.113550","DOIUrl":"10.1016/j.micromeso.2025.113550","url":null,"abstract":"<div><div>Nitrous oxide (N<sub>2</sub>O), the third most important greenhouse gas, is discharged from various anthropogenic sources and causes severe environmental problems. Herein, the natural mordenite zeolite is demonstrated to be an effective adsorbent to capture low-concentration N<sub>2</sub>O (below 30 ppm). An adsorption capacity of 0.076 mmol g<sup>−1</sup> can be achieved at −7 °C with 1 ppm N<sub>2</sub>O in the dynamic adsorption test, 6.3 times as high as that at 25 °C. The density functional theory calculations reveal that the Ca-exchanged MOR-type zeolite has stronger interactions with N<sub>2</sub>O compared with the Na-exchanged one. However, as evidenced by the isosteric adsorption enthalpy analysis and the Fourier transform infrared spectroscopy, the natural mordenite zeolite with both Na<sup>+</sup> and Ca<sup>2+</sup>, as well as the synthesized analogue, demonstrates stronger and distinctive interactions with trace N<sub>2</sub>O in comparison to the MOR-type zeolites with single kind of extra-framework cation. These results provide experimental and theoretical foundations for the establishment of efficient N<sub>2</sub>O removal system using well designed zeolite-based adsorbents under proper operating conditions.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"388 ","pages":"Article 113550"},"PeriodicalIF":4.8,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143445734","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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