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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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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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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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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

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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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Review of plasma-assisted reactions and potential applications for modification of metal–organic frameworks

Tingting Zhao, Niamat Ullah, Yajun Hui, Zhenhua Li

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 444-457 doi: 10.1007/s11705-019-1811-6

摘要： Plasma catalysis is drawing increasing attention worldwide. Plasma is a partially ionized gas comprising electrons, ions, molecules, radicals, and photons. Integration of catalysis and plasma can enhance catalytic activity and stability. Some thermodynamically unfavorable reactions can easily occur with plasma assistance. Compared to traditional thermal catalysis, plasma reactors can save energy because they can be operated at much lower temperatures or even room temperature. Additionally, the low bulk temperature of cold plasma makes it a good alternative for treatment of temperature-sensitive materials. In this review, we summarize the plasma-assisted reactions involved in dry reforming of methane, CO methanation, the methane coupling reaction, and volatile organic compound abatement. Applications of plasma for modification of metal–organic frameworks are discussed.

关键词： plasma catalysis     methane     carbon dioxide     VOCs     metal–organic frameworks    

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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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Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

《能源前沿（英文）》 2022年 第16卷 第5期   页码 734-746 doi: 10.1007/s11708-022-0840-x

摘要： This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal–organic framework (MOF)-based systems toward the photocatalytic hydrogen evolution (PHE) reaction through specific strategies: tailoring the photocatalytic activity of bare MOFs and guest@MOF composites, formation of heterojunctions based on MOFs and various photocatalysts, and inorganic photocatalysts derived from MOFs. According to the data reported in this mini-review, the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units (SBUs). Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view, many of these studies relate this activity to the physicochemical and catalytic properties of MOFs. However, they did not consider the interactions between the components of the photocatalytic material. This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE. A thorough review and comparison of the results established that metal–nanoparticle@MOF composites have weak van der Waals forces between components, whereas heterostructures only interact with MOFs at the surface of bare materials. Regarding material derivatives from MOFs, we found that pyrolysis destroyed some beneficial properties of MOFs for PHE. Thus, we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.

关键词： metal–organic frameworks (MOFs)     photocatalytic hydrogen evolution     MOF heterojunctions     materials derived from MOFs     bandgap     recombination    

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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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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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Construction of MOFs-based nanocomposite membranes for emerging organic contaminants abatement in water

《环境科学与工程前沿（英文）》 2023年 第17卷 第7期 doi: 10.1007/s11783-023-1689-x

摘要：

● Application of the MOF-composite membranes in adsorption was discussed.

关键词： Emerging organic contaminants     Metal organic frameworks     Synthesis     Adsorption     Catalysis    

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用于气体分离的含多孔材料的混合基质膜——从金属有机框架到离散分子笼 Review

杨子琪, 吴中杰, 白胜博, 应允攀, 杨昊, 赵丹

《工程（英文）》 2023年 第23卷 第4期   页码 40-55 doi: 10.1016/j.eng.2022.07.022

摘要：

混合基质膜（MMMs）将多孔材料与聚合物基质结合，因二者的互补性和协同作用，MMMs在气体分离研究领域得到了广泛关注。多孔材料的可调节性和多样性赋予了MMMs可扩展的功能和优异的分离性能。为了充分发挥MMMs的潜力，研究人员专注于多孔填料与聚合物基质的合理匹配，以提高MMMs的
界面相容性。在本文中，我们重点介绍了利用不同策略，将金属有机框架（MOFs）或金属有机笼（MOCs）与聚合物基质相结合，以制备MMMs的最新进展，并且进一步讨论了MMMs未来发展所面临的机遇和挑战，这将通过合理的材料设计和选择促进MMMs的发展。

关键词： 气体分离     金属-有机框架     金属-有机笼     混合基质膜     界面相容性    

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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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Fabrication of MIL-100(Fe)@SiO

Yinlong Hu,Shuang Zheng,Fumin Zhang

《化学科学与工程前沿（英文）》 2016年 第10卷 第4期   页码 534-541 doi: 10.1007/s11705-016-1596-9

摘要： Heterogeneous catalysts with convenient recyclability and reusability are vitally important to reduce the cost of catalysts as well as to avoid complex separation and recovery operations. In this regard, magnetic MIL-100(Fe)@SiO @Fe O microspheres with a novel core-shell structure were fabricated by the self-assembly of a metal-organic MIL-100(Fe) framework around pre-synthesized magnetic SiO @Fe O particles under relatively mild and environmentally benign conditions. The catalytic activity of the MIL-100(Fe)@SiO @Fe O catalyst was tested for the liquid-phase acetalization of benzaldehyde and glycol. The MIL-100(Fe)@SiO @Fe O catalyst has a significant amount of accessible Lewis acid sites and therefore exhibited good acetalization catalytic activity. Moreover, due to its superparamagnetism properties, the heterogeneous MIL-100(Fe)@SiO @Fe O catalyst can be easily isolated from the reaction system within a few seconds by simply using an external magnet. The catalyst could then be reused at least eight times without significant loss in catalytic efficiency.

关键词： metal-organic frameworks     heterogeneous catalysis     magnetically recoverable catalysts     core-shell structure     acetalization    

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标题 作者 时间 类型 操作

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

Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

期刊论文

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

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction

期刊论文

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

Zaiku Xie, Bao-Lian Su

期刊论文

Review of plasma-assisted reactions and potential applications for modification of metal–organic frameworks

Tingting Zhao, Niamat Ullah, Yajun Hui, Zhenhua Li

期刊论文

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

期刊论文

Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

期刊论文

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

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

Construction of MOFs-based nanocomposite membranes for emerging organic contaminants abatement in water

期刊论文

用于气体分离的含多孔材料的混合基质膜——从金属有机框架到离散分子笼

杨子琪, 吴中杰, 白胜博, 应允攀, 杨昊, 赵丹

期刊论文

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

期刊论文

Fabrication of MIL-100(Fe)@SiO

Yinlong Hu,Shuang Zheng,Fumin Zhang

期刊论文