Microporous and Mesoporous Materials最新文献

英文中文

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

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.

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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

New insights into the fluorine-alkali treatment and its application to ZSM-11 as a superior catalyst for chloromethane to propylene

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-15 DOI: 10.1016/j.micromeso.2025.113547

Ting Xu, Shiyu Cen, Qinghu Tang, Pengling Zhang, Qianyi Zhao, Jie Zhang

引用次数: 0

One-step synthesis of aluminum dross-derived MIL-53(Al) as an aniline adsorbent

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-15 DOI: 10.1016/j.micromeso.2025.113549

Ryota Yamane , Yuki Masuda , Satoshi Kobayashi , Hiroki Konno

Aluminum dross, an industrial waste product generated during the smelting and recycling of aluminum, is used in various industries; however, its application is limited. Metal–organic frameworks (MOFs), next-generation porous materials comprising metals and organic likers, offer tunable properties, including pore structure (shape and size), hydrophobicity, hydrophilicity, and stability, making them versatile for various applications. This study successfully achieved the one-step synthesis of MIL-53(Al), an MOF, using aluminum dross as a starting material for the first time. The dross-derived MIL-53(Al) exhibited high crystallinity, similar to that of conventional MIL-53(Al). It was further evaluated as an adsorbent for aniline, a compound widely used in chemical and pharmaceutical industries but harmful to human health and ecosystems. Liquid-phase adsorption experiments demonstrated that dross-derived MIL-53(Al) achieved an adsorption capacity similar to that of conventional MIL-53(Al), primarily owing to π‒π and hydrogen bonding interactions with aniline. The adsorption isotherm of dross-derived MIL-53(Al) conformed to the Langmuir model, indicating that the primary adsorption sites for aniline were its micropores. Furthermore, this MIL-53(Al) retained its adsorption capacity after up to four regeneration cycles using calcination. Thus, this study successfully synthesized MIL-53(Al) using aluminum dross as a precursor and demonstrated its potential effectiveness as a water purification agent.

{"title":"One-step synthesis of aluminum dross-derived MIL-53(Al) as an aniline adsorbent","authors":"Ryota Yamane , Yuki Masuda , Satoshi Kobayashi , Hiroki Konno","doi":"10.1016/j.micromeso.2025.113549","DOIUrl":"10.1016/j.micromeso.2025.113549","url":null,"abstract":"<div><div>Aluminum dross, an industrial waste product generated during the smelting and recycling of aluminum, is used in various industries; however, its application is limited. Metal–organic frameworks (MOFs), next-generation porous materials comprising metals and organic likers, offer tunable properties, including pore structure (shape and size), hydrophobicity, hydrophilicity, and stability, making them versatile for various applications. This study successfully achieved the one-step synthesis of MIL-53(Al), an MOF, using aluminum dross as a starting material for the first time. The dross-derived MIL-53(Al) exhibited high crystallinity, similar to that of conventional MIL-53(Al). It was further evaluated as an adsorbent for aniline, a compound widely used in chemical and pharmaceutical industries but harmful to human health and ecosystems. Liquid-phase adsorption experiments demonstrated that dross-derived MIL-53(Al) achieved an adsorption capacity similar to that of conventional MIL-53(Al), primarily owing to π‒π and hydrogen bonding interactions with aniline. The adsorption isotherm of dross-derived MIL-53(Al) conformed to the Langmuir model, indicating that the primary adsorption sites for aniline were its micropores. Furthermore, this MIL-53(Al) retained its adsorption capacity after up to four regeneration cycles using calcination. Thus, this study successfully synthesized MIL-53(Al) using aluminum dross as a precursor and demonstrated its potential effectiveness as a water purification agent.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"388 ","pages":"Article 113549"},"PeriodicalIF":4.8,"publicationDate":"2025-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143422317","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 surfactant-induced porosity and acidity modification of MOF-808 catalyst on the glycerol acetylation reaction

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-12 DOI: 10.1016/j.micromeso.2025.113539

César A. Bravo-Sanabria , Leidy C. Solano-Delgado , Daniela Rosas-Ardila , Carolina Ardila-Suárez , Víctor G. Baldovino-Medrano , Gustavo E. Ramírez-Caballero

A promising approach for the catalytic acetylation of glycerol to produce high value-added chemicals such as diacetins (DAGs) and triacetin (TAG) is the use of acidic Metal-Organic Frameworks (MOFs). Particularly, MOF-808 has shown potential as catalyst for this reaction due to its tunable porosity and the ability to incorporate acid sites. Herein, we focused on modifying the porosity and acidity of MOF-808 to improve its catalytic performance in the acetylation of glycerol. Porosity changes were induced during the synthesis of MOF-808 by promoting the formation of larger pores using three different surfactants: cetyltrimethylammonium bromide (CTAB), sodium dodecyl sulfate (SDS), and pluronic P123 (PLU), in combination with propionic acid as a modulator. Results showed that the proposed modifications add either mesoporosity; pores with widths larger than 2.0 nm, or macroporosity, i.e., pores with widths larger than 50.0 nm, when it is used surfactants, to the purely microporous MOF-808. On the other hand, the acidity of porosity enhanced MOF-808 was modified by a post-synthetic acid treatment with sulfuric acid. This treatment led to the incorporation of well dispersed sulfate groups into the MOF structure which did not experienced a strong loss of porosity. Catalytic experiments demonstrated that the sulfated MOF samples exhibited higher glycerol conversion if compared to the other samples, while the non-sulfated MOF modified with pluronic P123 showed the highest selectivity towards triacetin. This suggests that the improved accessibility provided by mesopores facilitates the sequential acetylation steps, particularly favoring the formation of triacetin as the final product.

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引用次数: 0

Corrigendum to “Facile synthesis of ordered mesoporous Cu-ZrPO with high copper contents as catalyst for liquid phase oxidation of ethylbenzene” [Microporous Mesoporous Mater. 198, 2014, 271–280]

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-08 DOI: 10.1016/j.micromeso.2025.113526

Zhichao Miao , Huahua Zhao , Jian Yang , Jun Zhao , Huanling Song , Lingjun Chou

引用次数: 0

Synthesis of spherical mesoporous silica beads with tunable size, stiffness and porosity

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials

Pub Date : 2025-02-06 DOI: 10.1016/j.micromeso.2025.113534

M. Milani , K. Ahmad , E. Cavalletti , C. Ligoure , L. Cipelletti , M. Kongkaew , P. Trens , L. Ramos

We present an innovative template-free water-based sol–gel method to produce uniform mesoporous silica beads of millimeter size, which have tunable size, stiffness and porosity, and could be used for adsorption applications. Our protocol exploits an in-situ enzymatic reaction to produce spherical beads of hydrogel from a charge-stabilized suspension of silica nanoparticles confined in a millimetric drop suspended in a non-miscible oil. Once the gelation step is complete, the spherical bead of gel is cleaned from oil and deposited onto a hydrophobic surface and let dry. Separating the gelation to the drying steps ensures a spatially uniform gel and allows us to perform a solvent exchange before drying. For all beads, we observe a crack-free drying process leading to the formation of stiff quasi-spherical beads with diameter in the range 1 to 5 mm and Young modulus in the range

(0.1 - 2) GPa

and narrow pore size distribution, centered around 10 to

25 nm

depending on the experimental conditions. Finally, to demonstrate the potentiality of these materials, we graft on the bead surface aminosilane molecules, and quantify their CO

_{2}

adsorption efficiency. Overall, the production method we have developed is simple, readily adaptable, and offers promising materials for adsorption, storage, catalysis and chromatography.

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引用次数: 0

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