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期刊论文 11

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绿色化工 1

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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    

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

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

《化学科学与工程前沿(英文)》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要: Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词: metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

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    

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    

Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation: a mini-review

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    

Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)

Ehsan Rahmani, Mohammad Rahmani

《化学科学与工程前沿(英文)》 2020年 第14卷 第6期   页码 1100-1111 doi: 10.1007/s11705-019-1891-3

摘要: A solvothermal method was used to synthesize MIL-101(Fe) and MIL-88(Fe), which were used for alkylation of benzene. The synthesized catalysts were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, field emission scanning electron microscope, dynamic light scattering, and BET techniques. Metal-organic frameworks (MOFs) were modeled to investigate the catalytic performance and existence of mass transfer limitations. Calculated effectiveness factors revealed absence of internal and external mass transfer. Sensitivity analysis revealed best operating conditions over MIL-101 at 120°C and 5 bar and over MIL-88 at 142°C and 9 bar.

关键词: MOFs     alkylation     ethylbenzene     catalysts pellet model     kinetic model     sensitivity analysis    

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    

Metal-organic framework-based CO

Yujie Ban, Meng Zhao, Weishen Yang

《化学科学与工程前沿(英文)》 2020年 第14卷 第2期   页码 188-215 doi: 10.1007/s11705-019-1872-6

摘要: A low-carbon economy calls for CO capture technologies. Membrane separations represent an energy-efficient and environment-friendly process compared with distillations and solvent absorptions. Metal-organic frameworks (MOFs), as a novel type of porous materials, are being generated at a rapid and growing pace, which provide more opportunities for high-efficiency CO capture. In this review, we illustrate a conceptional framework from material design and membrane separation application for CO capture, and emphasize two importance themes, namely (i) design and modification of CO -philic MOF materials that targets secondary building units, pore structure, topology and hybridization and (ii) construction of crack-free membranes through chemical epitaxy growth of active building blocks, interfacial assembly, ultrathin two-dimensional nanosheet assembly and mixed-matrix integration strategies, which would give rise to the most promising membrane performances for CO capture, and be expected to overcome the bottleneck of permeability-selectivity limitations.

关键词: CO2 capture     CO2-philic MOFs     crack-free membranes    

Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1389-1398 doi: 10.1007/s11705-022-2285-5

摘要: Hydrothermal and catalytic stability of UIO-66 MOFs with defective structures are critical aspects to be considered in their catalytic applications, especially under the conditions involving water, moisture and/or heat. Here, we report a facile strategy to introduce the macromolecular acid group to UIO-66 to improve the stability of the resulting UIO-66−PhSO3H MOF in aqueous phase catalysis. In detail, UIO-66−PhSO3H was obtained by grafting benzenesulfonic acid on the surface of the pristine UIO-66 to introduce the hydrophobicity, as well as the Brønsted acidity, then assessed using catalytic hydrolysis of cyclohexyl acetate (to cyclohexanol) in water. The introduction of hydrophobic molecules to UIO-66 could prevent the material from being attacked by hydroxyl polar molecules effectively, explaining its good structural stability during catalysis. UIO-66−PhSO3H promoted the conversion of cyclohexyl acetate at ca. 87%, and its activity and textural properties were basically intact after the cyclic stability tests. The facile modification strategy can improve the hydrothermal stability of UIO-66 significantly, which can expand its catalytic applications in aqueous systems.

关键词: metal−organic frameworks (MOFs)     UIO-66     hydrolysis of cyclohexyl acetate     hydrophobicity     Brønsted acidity    

In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytic hydrogen production

《能源前沿(英文)》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要: Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词: photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

标题 作者 时间 类型 操作

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

期刊论文

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

Zaiku Xie, Bao-Lian Su

期刊论文

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

期刊论文

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

期刊论文

Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

期刊论文

Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation: a mini-review

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

期刊论文

Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)

Ehsan Rahmani, Mohammad Rahmani

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

Metal-organic framework-based CO

Yujie Ban, Meng Zhao, Weishen Yang

期刊论文

Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

期刊论文

In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytic hydrogen production

期刊论文