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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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Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

《能源前沿（英文）》 2019年 第13卷 第2期   页码 221-250 doi: 10.1007/s11708-019-0629-8

摘要： Metal-organic frameworks (MOFs) have attracted much attention because of their large surface areas, tunable structures, and potential applications in many areas. In recent years, MOFs have shown much promise in CO photoreduction. This review summarized recent research progresses in MOF-based photocatalysts for photocatalytic reduction of CO . Besides, it discussed strategies in rational design of MOF-based photocatalysts (functionalized pristine MOFs, MOF-photosensitizer, MOF- semiconductor, MOF-metal, and MOF-carbon materials composites) with enhanced performance on CO reduction. Moreover, it explored challenges and outlook on using MOF-based photocatalysts for CO reduction.

关键词： metal-organic frameworks (MOFs)     photocatalysis     CO2 photoreduction     composite    

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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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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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Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要： Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词： MOF derivative     graphene     electrocatalyst     oxygen reduction reaction     oxygen evolution reaction     hydrogen evolution reaction    

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绿色化工应用导向的金属-有机框架材料研究概述 Review

孔祥婧, 李建荣

《工程（英文）》 2021年 第7卷 第8期   页码 1115-1139 doi: 10.1016/j.eng.2021.07.001

摘要：

快速的工业化进程导致当今全球性的能源和环境危机，以推动科技进步、解决相关挑战为目标，发展新型功能材料的重要性与日俱增。近年来，金属-有机框架（MOF）以及MOF衍生物材料引起了广泛关注，促使我们继续进行其结构设计和应用性能方面的探索。MOF材料的制备、表征和加工成型是实现其工业应用的基础。研究人员已经围绕这些主题开展了大量的工作，以绿色化工应用为导向，充分发挥功能性优势，推动MOF材料大规模的工业应用也应当被提上日程。在解决实际问题的过程中，许多经典MOF表现出了相对传统材料的优越性。文中将从MOF化学中的基本概念出发，讨论了MOF材料的工业合成进展及其在多个领域中的应用现状，旨在提供一个系统的研究概述，引导研究者逐渐将研究思路从学术研究转向实际应用。在成本、规模化生产、加工成型和稳定性等挑战被逐一突破之后，MOF及其衍生物材料有望走进工厂，成为我们日常生活中的一部分，进而为人类创造一个基于绿色生产和生活方式的新时代。

关键词： 金属-有机框架     应用     绿色化工    

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A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

《化学科学与工程前沿（英文）》   页码 1632-1642 doi: 10.1007/s11705-022-2187-6

摘要： Although metal–organic frameworks offer a new platform for developing versatile sorption materials, yet coordinating the functionality, structure and component of these materials remains a great challenge. It depends on a comprehensive knowledge of a “real sorption mechanism”. Herein, a ternary mechanism for U(VI) uptake in metal–organic frameworks was reported. Analogous MIL-100s (Al, Fe, Cr) were prepared and studied for their ability to sequestrate U(VI) from aqueous solutions. As a result, MIL-100(Al) performed the best among the tested materials, and MIL-100(Cr) performed the worst. The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(VI) uptake in the three metal–organic frameworks involves different mechanisms. Specifically, hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s (Al, Fe) by exchanging with hydrogen ions of terminal hydroxyl groups (Al-OH2, Fe-OH2), and/or, hydrated uranyl ions are bound directly to Al(III) center in MIL-100(Al) through a strong inner-sphere coordination. For MIL-100(Cr), however, the U(VI) uptake is attributed to electrostatic attraction. Besides, the sorption mechanism is also pH and ionic strength dependent. The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism, which helps to construct effective metal–organic frameworks-based sorbents for water purification.

关键词： U(VI)     metal–organic frameworks     adsorption mechanism     metal node    

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Selective capture and separation of xenon and krypton using metal organic frameworks: a review

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1895-1912 doi: 10.1007/s11705-023-2355-3

摘要： Xenon and krypton are widespread useful noble gases in commercial lighting, lasers, electronics, and medical industry. At the same time, radioactive noble gases may proliferate from used nuclear fuel and diffuse in open atmospheres. Metal organic frameworks as hotspot porous materials for gases uptake and separation are considered to be potential solutions. In this review, we comprehensively summarized recent researches on metal organic frameworks for selective capture and separation of xenon and krypton. Particularly, we followed the aspects of different optimal design strategies, including optimal pore/cage size and geometry, open metal sites, ions (anions and cations), and polar functional groups for enhancing the xenon adsorption and separation performances. Meanwhile, a comparison of each strategy and the mechanisms of xenon/krypton separation were pointed out. The separation of krypton from gases mixtures by dual-bed systems was further discussed. Finally, some existing challenges and opportunities for possible real applications were proclaimed.

关键词： metal organic frameworks     xenon     krypton     selective separation     used nuclear fuel    

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Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

《能源前沿（英文）》 2021年 第15卷 第3期   页码 656-666 doi: 10.1007/s11708-021-0765-9

摘要： In recent years, defect-engineered Zr-based UiO-66 metal-organic frameworks (UiO-66(Zr) metal-organic frameworks (MOFs)) have shown huge advantages in catalytic, functional materials, adsorption, and other fields due to their large surface areas, well-ordered porous structures, and flexible tailorability. It is extremely challenging to introduce defect sites in the synthesis of MOFs to regulate the physicochemical properties of materials such as (energy band structure, pore structure, etc.) to obtain an excellent performance. This paper reviews the recent research results of synthesis methods, characterization technologies, and application fields of defect-engineered UiO-66(Zr) MOFs materials in order to provide new insights to synthesize high-performance UiO-66(Zr) MOFs materials and promote the development of UiO-66(Zr) in various fields.

关键词： defect engineering     metal-organic frameworks     UiO-66     photocatalysis    

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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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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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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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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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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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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

Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

期刊论文

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

期刊论文

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

Zaiku Xie, Bao-Lian Su

期刊论文

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient

期刊论文

绿色化工应用导向的金属-有机框架材料研究概述

孔祥婧, 李建荣

期刊论文

A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

期刊论文

Selective capture and separation of xenon and krypton using metal organic frameworks: a review

期刊论文

Research progress of defect-engineered UiO-66(Zr) MOFs for photocatalytic hydrogen production

期刊论文

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

期刊论文

Metal-organic framework UiO-66 membranes

Xinlei Liu

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

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

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