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Hierarchical porous metal-organic frameworks/polymer microparticles for enhanced catalytic degradationof organic contaminants

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 939-949 doi: 10.1007/s11705-022-2152-4

摘要： This work reports on a simple microfluidic strategy to controllably fabricate uniform polymeric microparticles containing hierarchical porous structures integrated with highly accessible catalytic metal organic frameworks for efficient degradation of organic contaminants. Monodisperse (W1/O)/W2 emulsion droplets generated from microfluidics are used as templates for the microparticle synthesis. The emulsion droplets contain tiny water microdroplets from homogenization and water nanodroplets from diffusion-induced swollen micelles as the dual pore-forming templates, and Fe-based metal-organic framework nanorods as the nanocatalysts. The obtained microparticles possess interconnected hierarchical porous structures decorated with highly accessible Fe-based metal-organic framework nanorods for enhanced degradation of organic contaminants via a heterogeneous Fenton-like reaction. Such a degradation performance is highlighted by using these microparticles for efficient degradation of rhodamine B in hydrogen peroxide solution. This work provides a simple and general strategy to flexibly combine hierarchical porous structures and catalytic metal-organic frameworks to engineer advanced microparticles for water decontamination.

关键词： metal-organic framework     polymer microparticle     nanocatalyst     decontamination     organic contaminant    

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Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 395-403 doi: 10.1007/s11705-022-2218-3

摘要： Radioactive iodine exhibits medical values in radiology, but its excessive emissions can cause environmental pollution. Thus, the capture of radioiodine poses significant engineering for the environment and medical radiology. The adsorptive capture of radioactive iodine by metal–organic frameworks (MOFs) has risen to prominence. In this work, a Th-based MOF (denoted as Th-BPYDC) was structurally designed and synthesized, consisting of [Th6(μ3-O)4(μ3-OH)4(H2O)6]12+ clusters, abundant bipyridine units, and large cavities that allowed guest molecules diffusion and transmission. Th-BPYDC exhibited the uptake capacities of 2.23 g·g−1 and 312.18 mg·g−1 towards I2 vapor and I2 dissolved in cyclohexane, respectively, surpassing its corresponding analogue Th-UiO-67. The bipyridine units boosted the adsorption performance, and Th-BPYDC showed good reusability with high stability. Our work thus opened a new way for the synthesis of MOFs to capture radioactive iodine.

关键词： metal–organic framework     iodine     adsorption     nuclear waste     environmental remediation    

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Metal-organic framework UiO-66 membranes

Xinlei Liu

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 216-232 doi: 10.1007/s11705-019-1857-5

摘要： Metal-organic frameworks (MOFs) have emerged as a class of promising membrane materials. UiO-66 is a prototypical and stable MOF material with a number of analogues. In this article, we review five approaches for fabricating UiO-66 polycrystalline membranes including synthesis, secondary synthesis, biphase synthesis, gas-phase deposition and electrochemical deposition, as well as their applications in gas separation, pervaporation, nanofiltration and ion separation. On this basis, we propose possible methods for scalable synthesis of UiO-66 membranes and their potential separation applications in the future.

关键词： membrane     metal-organic framework     UiO-66     separation    

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Fluorescence detection of phosphate in an aqueous environment by an aluminum-based metal-organic framework

《环境科学与工程前沿（英文）》 2022年 第16卷 第12期 doi: 10.1007/s11783-022-1594-8

摘要：

● A novel Al-MOF was successfully synthesized by a facile solvothermal method.

关键词： Fluorescence     Metal-organic framework     Phosphate     Detection     Al-MOF    

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Nickel-based metal−organic framework-derived whisker-shaped nickel phyllosilicate toward efficiently

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1493-1504 doi: 10.1007/s11705-022-2168-9

摘要： Metal−organic framework-derived materials have attracted significant attention in the applications of functional materials. In this work, the rod-like nickel-based metal−organic frameworks were first synthesized and subsequently employed as the hard templates and nickel sources to prepare the whisker-shaped nickel phyllosilicate using a facile hydrothermal technology. Then, the nickel phyllosilicate whiskers were evaluated to enhance the mechanical, thermal, flammable, and tribological properties of epoxy resin. The results show that adequate nickel phyllosilicate whiskers can disperse well in the matrix, improving the tensile strength and elastic modulus by 13.6% and 56.4%, respectively. Although the addition of nickel phyllosilicate whiskers could not obtain any UL-94 ratings, it enhanced the difficulty in burning the resulted epoxy resin nanocomposites and considerably enhanced thermal stabilities. Additionally, it was demonstrated that such nickel phyllosilicate whiskers preferred to improve the wear resistance instead of the antifriction feature. Moreover, the wear rate of epoxy resin nanocomposites was reduced significantly by 80% for pure epoxy resin by adding 1 phr whiskers. The as-prepared nickel phyllosilicate whiskers proved to be promising reinforcements in preparing of high-performance epoxy resin nanocomposites.

关键词： metal−organic framework     nickel phyllosilicate     whisker     epoxy resin     mechanical response     tribological performance     flammable property    

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A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

《环境科学与工程前沿（英文）》 2023年 第17卷 第3期 doi: 10.1007/s11783-023-1633-0

摘要：

● pz-UiO-66 was synthesized facilely by a solvothermal method.

关键词： Pyrazine     Metal-organic frameworks     Copper removal     Strong acidity     High selectivity    

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Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1139-1148 doi: 10.1007/s11705-021-2111-5

摘要： The solubility of Pd(NO3)2 in water is moderate whereas it is completely soluble in diluted HNO3 solution. Pd/MIL-101(Cr) and Pd/MIL-101-NH2(Cr) were synthesized by aqueous solution of Pd(NO3)2 and Pd(NO3)2 solution in dilute HNO3 and used for CO oxidation reaction. The catalysts synthesized with Pd(NO3)2 solution in dilute HNO3 showed lower activity. The aqueous solution of Pd(NO3)2 was used for synthesis of mono-metal Ni, Pd and bimetallic PdNi nanoparticles with various molar ratios supported on MOF. Pd70Ni30/MIL-101(Cr) catalyst showed higher activity than monometallic counterparts and Pd+ Ni physical mixture due to the strong synergistic effect of PdNi nanoparticles, high distribution of PdNi nanoparticles, and lower dissociation and desorption barriers. Comparison of the catalysts synthesized by MIL-101(Cr) and MIL-101-NH2(Cr) as the supports of metals showed that Pd/MIL-101-NH2(Cr) outperforms Pd/MIL-101-(Cr) because of the higher electron density of Pd resulting from the electron donor ability of the NH2 functional group. However, the same activities were observed for Pd70Ni30/MIL-101(Cr) and Pd70Ni30/MIL-101-NH2(Cr), which is due to a less uniform distribution of Pd nanoparticles in Pd70Ni30/MIL-101-NH2(Cr) originated from amorphization of MIL-101-NH2(Cr) structure during the reduction process. In contrast, Pd70Ni30/MIL-101(Cr) revealed the stable structure and activity during reduction and CO oxidation for a long time.

关键词： CO oxidation     heterogeneous catalysis     metal-organic framework     NH2 functional group     PdNi    

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Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 123-126 doi: 10.1007/s11705-020-1921-1

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Engineering zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 511-522 doi: 10.1007/s11705-021-2068-4

摘要： Lithium-sulfur batteries have been regarded as the next-generation rechargeable batteries due to their high theoretical energy density and specific capacity. Nevertheless, the shuttle effect of lithium polysulfides has hindered the development of lithium-sulfur batteries. Herein, a novel zirconium-based metal-organic framework-801 film on carbon cloth was developed as a versatile interlayer for lithium-sulfur batteries. This interlayer has a hierarchical porous structure, suitable for the immobilization of lithium polysulfides and accommodating volume expansion on cycling. Moreover, the MOF-801 material is capable of strongly adsorbing lithium polysulfides and promoting their catalytic conversion, which can be enhanced by the abundant active sites provided by the continuous structure of the MOF-801 films. Based on the above advantages, the lithium-sulfur battery, with the proposed interlayer, delivers an initial discharge capacity of 927 mAh·g–1 at 1 C with an extremely low decay rate of 0.04% over 500 cycles. Additionally, a high area capacity of 4.3 mAh·cm–2 can be achieved under increased S loading.

关键词： lithium-sulfur batteries     metal-organic framework-801 film     interlayer     shuttle effect    

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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H2), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes     room-temperature hydrogenation     Ni nanoparticles     nitrogen-doped carbon nanoneedles     metal–organic-framework    

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Hydrophobic nanocellulose aerogels with high loading of metal-organic framework particles as floating

Jiajia Li, Shengcheng Zhai, Weibing Wu, Zhaoyang Xu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1158-1168 doi: 10.1007/s11705-020-2021-z

摘要： In this paper, we employed a facile approach to prepare flexible and porous metal-organic frameworks (MOFs) containing cellulose nanofiber (CNF) aerogels (MNCAs) through freeze-drying MOF-containing cellulose nanofiber suspensions. After coating with methyltrimethoxysilane (MTMS) by chemical vapor deposition, recycled and hydrophobic MTMS-coated MNCAs (MMNCAs) were obtained. Due to the low density (0.009 g/cm ), high porosity (97%) and good mechanical properties of the aerogel, the adsorption capacity of MMNCAs reached up to 210 g/g, which was nearly 3‒5 times that of pure CNF aerogels. These prepared aerogels showed excellent oil/water selectivity and high capacity to adsorb oil and organic solvents. This kind of cellulose-based aerogel may be applicable in the field of environmental protection.

关键词： cellulose nanofibers     aerogels     metal-organic framework     oil-adsorption    

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Integrating of metal-organic framework UiO-66-NH2 and cellulose nanofibers mat for high-performance adsorption

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1387-1398 doi: 10.1007/s11705-022-2154-2

摘要： UiO-66-NH2 is an efficient material for removing pollutants from wastewater due to its high specific surface area, high porosity and water stability. However, recycling them from wastewater is difficult. In this study, the cellulose nanofibers mat deacetylated from cellulose acetate nanofibers were used to combine with UiO-66-NH2 by the method of in-situ growth to remove the toxic dye, rose bengal. Compared to previous work, the prepared composite could not only provide ease of separation of UiO-66-NH2 from the water after adsorption but also demonstrate better adsorption capacity (683 mg∙g‒1 (T = 25 °C, pH = 3)) than that of the simple UiO-66-NH2 (309.6 mg∙g‒1 (T = 25 °C, pH = 3)). Through the analysis of adsorption kinetics and isotherms, the adsorption for rose bengal is mainly suitable for the pseudo-second-order kinetic model and Freundlich model. Furthermore, the relevant research revealed that the main adsorption mechanism of the composite was electrostatic interaction, hydrogen bonding and π–π interaction. Overall, the approach depicts an efficient model for integrating metal-organic frameworks on cellulose nanofibers to improve metal-organic framework recovery performance with potentially broad applications.

关键词： UiO-66-NH2     cellulose nanofibers     rose bengal     adsorption     mechanism    

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Tuning the primary selective nanochannels of MOF thin-film nanocomposite nanofiltration membranes for efficient removal of hydrophobic endocrine disrupting compounds

《环境科学与工程前沿（英文）》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1474-7

摘要：

• PA layer properties tune the primary nanochannels in MIL-101(Cr) TFN NF membranes.

关键词： Porous metal organic framework     Thin-film nanocomposite membrane     Primary selective nanochannels     Nanofiltration     Endocrine disrupting compounds    

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Metal-organic framework loaded manganese oxides as efficient catalysts for low-temperature selective

Minhua Zhang, Baojuan Huang, Haoxi Jiang, Yifei Chen

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 594-602 doi: 10.1007/s11705-017-1668-5

摘要： A mild deposition method was used to fabricate Mn-based catalysts on a UiO-66 carrier for the selective catalytic reduction of NO by NH (NH -SCR). The catalyst with 8.5 wt-% MnO loading had the highest catalytic activity for NH -SCR with a wide temperature window (100–290 °C) for 90% NO conversion. Characterization of the prepared MnO /UiO-66 catalysts showed that the catalysts had the crystal structure and porosity of the UiO-66 carrier and that the manganese particles were well-distributed on the surface of the catalyst. X-ray photoelectron spectroscopy analysis showed that there are strong interactions between the MnO and the Zr oxide secondary building units of the UiO-66 which has a positive effect on the catalytic activity. The 8.5 wt-% MnO catalyst maintained excellent activity during a 24-h stability test and exhibited good resistance to SO poisoning.

关键词： metal-organic framework     selective catalytic reduction     manganese oxides     deNOx     SO2 resistance    

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氢气分离膜研究进展

栾永超,熊亚林,何广利,刘聪敏,李帅

《中国工程科学》 2022年 第24卷 第3期   页码 140-152 doi: 10.15302/J-SSCAE-2022.03.015

摘要：

氢气是重要的工业原料和清洁燃料，氢气分离具有重要的经济和社会价值；膜分离法装置结构简单、转换高效、投资成本低且环境友好，在氢气分离领域应用前景广阔；氢气分离膜的性能是影响氢气分离过程效率的决定性因素，因而氢气分离膜技术研究一直是国内外膜领域的热点方向。本文阐述了氢气分离膜的应用需求、基本机理，系统梳理了致密金属膜、无机多孔膜、金属‒ 有机框架（MOF）膜、有机聚合物膜、混合基质膜的研究进展。研究发现，尽管无机多孔膜、有机聚合物膜、混合基质膜等具有良好的氢气分离纯化性能，但在分布式、小型化的应用场景下的分离性能仍待改进提高；提高钯基金属膜的抗毒化性能、优化膜的性价比，是促进工业应用的有效手段；整合无机多孔膜、MOF膜的优点，可促进分子筛分机制膜的性能跃升；有机聚合物膜的耐温、机械等性能仍需提高；对现有高分子膜材料进行改性、制备高分子合金，是开发新型气体分离膜的重要方向；混合基质膜在进行可控调节排布后，将显著提高膜性能。多种氢气分离膜的研究和应用，支撑了氢气分离纯化过程的发展，在材料种类丰富、制备工艺进步后将发挥更大的工程价值。

关键词： 氢气分离膜；致密金属膜；无机多孔膜；金属‒ 有机框架膜；有机聚合物膜；混合基质膜；氢气纯化    

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标题 作者 时间 类型 操作

Hierarchical porous metal-organic frameworks/polymer microparticles for enhanced catalytic degradationof organic contaminants

期刊论文

Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

期刊论文

Metal-organic framework UiO-66 membranes

Xinlei Liu

期刊论文

Fluorescence detection of phosphate in an aqueous environment by an aluminum-based metal-organic framework

期刊论文

Nickel-based metal−organic framework-derived whisker-shaped nickel phyllosilicate toward efficiently

期刊论文

A pyrazine based metal-organic framework for selective removal of copper from strongly acidic solutions

期刊论文

Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

期刊论文

Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

期刊论文

Engineering zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers

期刊论文

Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed

期刊论文

Hydrophobic nanocellulose aerogels with high loading of metal-organic framework particles as floating

Jiajia Li, Shengcheng Zhai, Weibing Wu, Zhaoyang Xu

期刊论文

Integrating of metal-organic framework UiO-66-NH2 and cellulose nanofibers mat for high-performance adsorption

期刊论文

Tuning the primary selective nanochannels of MOF thin-film nanocomposite nanofiltration membranes for efficient removal of hydrophobic endocrine disrupting compounds

期刊论文

Metal-organic framework loaded manganese oxides as efficient catalysts for low-temperature selective

Minhua Zhang, Baojuan Huang, Haoxi Jiang, Yifei Chen

期刊论文

氢气分离膜研究进展

栾永超,熊亚林,何广利,刘聪敏,李帅

期刊论文