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Advanced Metal-Organic Frameworks
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Advanced Metal-Organic Frameworks

A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Inorganic Materials and Metal-Organic Frameworks".

Deadline for manuscript submissions: closed (31 December 2022) | Viewed by 21188

Special Issue Editor

Prof. Dr. Fei Wang

E-Mail Website
Guest Editor
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, The Chinese Academy of Sciences, Fuzhou 350002, China
Interests: design and synthesis of zeolite-like metal–organic frameworks (MOFs); homochiral MOFs; Ti-MOF-based photocatalysts and/or electrocatalysts for gas separation; enantiomeric resolution; asymmetric catalysis; photoelectrocatalysis

Special Issue Information

Dear Colleagues,

Metal–organic frameworks (MOFs) are a new type of crystalline porous material. After more than 20 years of development, tens of thousands of MOFs have been synthesized which exhibit wide potential applications in adsorption and separation, luminescence, catalysis, biomedicine, and other fields. Especially in the biomedical field, because of its controllable pore size, functional groups and good biocompatibility, the preparation of nano-scale metal–organic framework materials for slow drug release and metabolism in living cells, real-time monitoring of life activities, etc., has great biological significance for people to understand important life activities in living organisms (such as the function of protein and the interaction between protein), to regulate the activation mechanism of protein, and to regulate the protein pathway related to major diseases. Therefore, developing multifunctional MOFs and MOF-based composite materials and applying them to different fields will greatly promote the mutual development of disciplines.

This Special Issue of Nanomaterials will aim to cover the latest development of metal–organic framework nanostructures, not only involving material synthesis, characterization, and multilevel assembly structure, but also reporting on their functions in thin film preparation and processing devices, including but not limited to gas adsorption and separation, biomedicine and drug delivery, photoelectrocatalysis, gas sensing, pollutant degradation and capture, and so on.

Prof. Dr. Fei Wang
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Nanomaterials is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2900 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • MOFs
  • Film
  • Gas separation
  • Gas sensing
  • Catalysis

Published Papers (8 papers)

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Research

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16 pages, 3890 KiB  
Article
Hydrocarbon Sorption in Flexible MOFs—Part II: Understanding Adsorption Kinetics
by Hannes Preißler-Kurzhöfer, Andrei Kolesnikov, Marcus Lange, Jens Möllmer, Oliver Erhart, Merten Kobalz, Seungtaik Hwang, Christian Chmelik, Harald Krautscheid and Roger Gläser
Nanomaterials 2023, 13(3), 601; https://doi.org/10.3390/nano13030601 - 02 Feb 2023
Cited by 2 | Viewed by 1419
Abstract
The rate of sorption of n-butane on the structurally flexible metal-organic framework [Cu2(H-Me-trz-ia)2], including its complete structural transition between a narrow-pore phase and a large-pore phase, was studied by sorption gravimetry, IR spectroscopy, and powder X-ray diffraction at [...] Read more.
The rate of sorption of n-butane on the structurally flexible metal-organic framework [Cu2(H-Me-trz-ia)2], including its complete structural transition between a narrow-pore phase and a large-pore phase, was studied by sorption gravimetry, IR spectroscopy, and powder X-ray diffraction at close to ambient temperature (283, 298, and 313 K). The uptake curves reveal complex interactions of adsorption on the outer surface of MOF particles, structural transition, of which the overall rate depends on several factors, including pressure step, temperature, as well as particle size, and the subsequent diffusion into newly opened pores. With the aid of a kinetic model based on the linear driving force (LDF) approach, both rates of diffusion and structural transition were studied independently of each other. It is shown that temperature and applied pressure steps have a strong effect on the rate of structural transition and thus, the overall velocity of gas uptake. For pressure steps close to the upper boundary of the gate-opening, the rate of structural transition is drastically reduced. This feature enables a fine-tuning of the overall velocity of sorption, which can even turn into anti-Arrhenius behavior. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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30 pages, 7456 KiB  
Article
Sr(II) and Ba(II) Alkaline Earth Metal–Organic Frameworks (AE-MOFs) for Selective Gas Adsorption, Energy Storage, and Environmental Application
by Nikolas Király, Dominika Capková, Róbert Gyepes, Nikola Vargová, Tomáš Kazda, Jozef Bednarčík, Daria Yudina, Tomáš Zelenka, Pavel Čudek, Vladimír Zeleňák, Anshu Sharma, Vera Meynen, Virginie Hornebecq, Andrea Straková Fedorková and Miroslav Almáši
Nanomaterials 2023, 13(2), 234; https://doi.org/10.3390/nano13020234 - 04 Jan 2023
Cited by 9 | Viewed by 2075
Abstract
Two new alkaline earth metal–organic frameworks (AE-MOFs) containing Sr(II) (UPJS-15) or Ba(II) (UPJS-16) cations and extended tetrahedral linker (MTA) were synthesized and characterized in detail (UPJS stands for University of Pavol Jozef Safarik). Single-crystal X-ray analysis (SC-XRD) revealed that [...] Read more.
Two new alkaline earth metal–organic frameworks (AE-MOFs) containing Sr(II) (UPJS-15) or Ba(II) (UPJS-16) cations and extended tetrahedral linker (MTA) were synthesized and characterized in detail (UPJS stands for University of Pavol Jozef Safarik). Single-crystal X-ray analysis (SC-XRD) revealed that the materials are isostructural and, in their frameworks, one-dimensional channels are present with the size of ~11 × 10 Å2. The activation process of the compounds was studied by the combination of in situ heating infrared spectroscopy (IR), thermal analysis (TA) and in situ high-energy powder X-ray diffraction (HE-PXRD), which confirmed the stability of compounds after desolvation. The prepared compounds were investigated as adsorbents of different gases (Ar, N2, CO2, and H2). Nitrogen and argon adsorption measurements showed that UPJS-15 has SBET area of 1321 m2 g−1 (Ar) / 1250 m2 g−1 (N2), and UPJS-16 does not adsorb mentioned gases. From the environmental application, the materials were studied as CO2 adsorbents, and both compounds adsorb CO2 with a maximum capacity of 22.4 wt.% @ 0 °C; 14.7 wt.% @ 20 °C and 101 kPa for UPJS-15 and 11.5 wt.% @ 0°C; 8.4 wt.% @ 20 °C and 101 kPa for UPJS-16. According to IAST calculations, UPJS-16 shows high selectivity (50 for CO2/N2 10:90 mixture and 455 for CO2/N2 50:50 mixture) and can be applied as CO2 adsorbent from the atmosphere even at low pressures. The increased affinity of materials for CO2 was also studied by DFT modelling, which revealed that the primary adsorption sites are coordinatively unsaturated sites on metal ions, azo bonds, and phenyl rings within the MTA linker. Regarding energy storage, the materials were studied as hydrogen adsorbents, but the materials showed low H2 adsorption properties: 0.19 wt.% for UPJS-15 and 0.04 wt.% for UPJS-16 @ −196 °C and 101 kPa. The enhanced CO2/H2 selectivity could be used to scavenge carbon dioxide from hydrogen in WGS and DSR reactions. The second method of applying samples in the area of energy storage was the use of UPJS-15 as an additive in a lithium-sulfur battery. Cyclic performance at a cycling rate of 0.2 C showed an initial discharge capacity of 337 mAh g−1, which decreased smoothly to 235 mAh g−1 after 100 charge/discharge cycles. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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19 pages, 13058 KiB  
Article
Transformation of Amorphous Terbium Metal–Organic Framework on Terbium Oxide TbOx(111) Thin Film on Pt(111) Substrate: Structure of TbxOy Film
by Helena Brunckova, Erika Mudra, Magdalena Streckova, Lubomir Medvecky, Tibor Sopcak, Ivan Shepa, Alexandra Kovalcikova, Maksym Lisnichuk and Hristo Kolev
Nanomaterials 2022, 12(16), 2817; https://doi.org/10.3390/nano12162817 - 17 Aug 2022
Cited by 5 | Viewed by 1784
Abstract
The present study is focused on the synthesis and structural properties of amorphous terbium metal–organic framework thin film (TbMOF-TF) and its transformation to terbium oxide by pyrolysis at 450 °C in the air. The crystalline (cTbMOF) and amorphous (aTbMOF) films were prepared by [...] Read more.
The present study is focused on the synthesis and structural properties of amorphous terbium metal–organic framework thin film (TbMOF-TF) and its transformation to terbium oxide by pyrolysis at 450 °C in the air. The crystalline (cTbMOF) and amorphous (aTbMOF) films were prepared by solvothermal synthesis using different amounts (0.4 and 0.7 mmol) of the modulator (sodium acetate), respectively. The powders were characterized by differential scanning calorimetry (DSC), thermogravimetry (TG), Fourier transform infrared (FTIR), Raman spectroscopy, and scanning electron microscopy (SEM). The varied chemical composition of the surface of TbMOFs and TbxOy was investigated by X-ray photoelectron spectroscopy (XPS). X-ray diffraction (XRD) and transmission electron microscopy (TEM) revealed that aTbMOF had been fully transformed to a Tb4O7 phase with a cubic crystal structure at 450 °C. The amorphous aTbMOF-TF film was prepared by dropping a colloidal solution of amorphous precursor nanocrystals on the SiO2/Si substrates covered with Pt as an interlayer. XPS confirmed the presence of Tb in two states, Tb3+ and Tb4+. The amorphous film has a rough, porous microstructure and is composed of large clusters of worm-like particles, while terbium oxide film consists of fine crystallites of cubic fluorite cF-TbOx, c-Tb4O7, and c-Tb2O3 phases. The surface topography was investigated by a combination of confocal (CM) and atomic force microscopy (AFM). The amorphous film is porous and rough, which is contrast to the crystalline terbium oxide film. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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12 pages, 2906 KiB  
Article
A Facile and General Approach to Enhance Water Resistance of Metal-Organic Frameworks by the Post-Modification with Aminopropyltriethoxylsilane
by Jianmei Gu, Jianquan Li and Qingyu Ma
Nanomaterials 2022, 12(7), 1134; https://doi.org/10.3390/nano12071134 - 29 Mar 2022
Cited by 3 | Viewed by 2171
Abstract
The water sensitivity of metal-organic frameworks (MOFs) as a common and crucial issue has greatly hindered their practical applications. Here, we present a facile and general approach to improve the water resistance of a typical MOF, i.e., CuBTC [Cu3(BTC)2(H [...] Read more.
The water sensitivity of metal-organic frameworks (MOFs) as a common and crucial issue has greatly hindered their practical applications. Here, we present a facile and general approach to improve the water resistance of a typical MOF, i.e., CuBTC [Cu3(BTC)2(H2O)3]n (BTC = benzene-1,3,5-tricarboxylate) using a post-modification reaction with aminopropyltriethoxylsilane (APTES) at room temperature. The afforded material is denoted as CuBTC@APTES. Various spectroscopic methods reveal that the organosilicon linkers have been successfully grafted onto CuBTC by electrostatic attraction between acid and base groups and without affecting the original coordination mode and basic structure. Compared with CuBTC, the water stability of CuBTC@APTES was significantly improved. The pristine CuBTC almost lost all its crystallinity, morphology and pore structure after 3-day treatment in water, while CuBTC@APTES is able to retain its main crystal structure and basic porosity after the same treatment. This finding can be explained by the successful introduction of the organosilicon molecular overlayer on the periphery of CuBTC to slow down the destruction of weak metal coordination bonds by water molecules, thus improving the water stability of CuBTC. The solution of water sensitivity provides more opportunities for the practical applications of CuBTC, such as aqueous phase catalysis and gas separation in humid environments. This simple approach can certainly be expanded to improve the water resistance of other carboxylate-containing ligand-based MOFs. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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14 pages, 4922 KiB  
Article
Machine Learning-Assisted Computational Screening of Metal-Organic Frameworks for Atmospheric Water Harvesting
by Lifeng Li, Zenan Shi, Hong Liang, Jie Liu and Zhiwei Qiao
Nanomaterials 2022, 12(1), 159; https://doi.org/10.3390/nano12010159 - 03 Jan 2022
Cited by 9 | Viewed by 3021
Abstract
Atmospheric water harvesting by strong adsorbents is a feasible method of solving the shortage of water resources, especially for arid regions. In this study, a machine learning (ML)-assisted high-throughput computational screening is employed to calculate the capture of H2O from N [...] Read more.
Atmospheric water harvesting by strong adsorbents is a feasible method of solving the shortage of water resources, especially for arid regions. In this study, a machine learning (ML)-assisted high-throughput computational screening is employed to calculate the capture of H2O from N2 and O2 for 6013 computation-ready, experimental metal-organic frameworks (CoRE-MOFs) and 137,953 hypothetical MOFs (hMOFs). Through the univariate analysis of MOF structure-performance relationships, Qst is shown to be a key descriptor. Moreover, three ML algorithms (random forest, gradient boosted regression trees, and neighbor component analysis (NCA)) are applied to hunt for the complicated interrelation between six descriptors and performance. After the optimizing strategy of grid search and five-fold cross-validation is performed, three ML can effectively build the predictive model for CoRE-MOFs, and the accuracy R2 of NCA can reach 0.97. In addition, based on the relative importance of the descriptors by ML, it can be quantitatively concluded that the Qst is dominant in governing the capture of H2O. Besides, the NCA model trained by 6013 CoRE-MOFs can predict the selectivity of hMOFs with a R2 of 0.86, which is more universal than other models. Finally, 10 CoRE-MOFs and 10 hMOFs with high performance are identified. The computational screening and prediction of ML could provide guidance and inspiration for the development of materials for water harvesting in the atmosphere. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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Review

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43 pages, 10323 KiB  
Review
BioMOF-Based Anti-Cancer Drug Delivery Systems
by Sandy Elmehrath, Ha L. Nguyen, Sherif M. Karam, Amr Amin and Yaser E. Greish
Nanomaterials 2023, 13(5), 953; https://doi.org/10.3390/nano13050953 - 06 Mar 2023
Cited by 13 | Viewed by 3453
Abstract
A variety of nanomaterials have been developed specifically for biomedical applications, such as drug delivery in cancer treatment. These materials involve both synthetic and natural nanoparticles and nanofibers of varying dimensions. The efficacy of a drug delivery system (DDS) depends on its biocompatibility, [...] Read more.
A variety of nanomaterials have been developed specifically for biomedical applications, such as drug delivery in cancer treatment. These materials involve both synthetic and natural nanoparticles and nanofibers of varying dimensions. The efficacy of a drug delivery system (DDS) depends on its biocompatibility, intrinsic high surface area, high interconnected porosity, and chemical functionality. Recent advances in metal-organic framework (MOF) nanostructures have led to the achievement of these desirable features. MOFs consist of metal ions and organic linkers that are assembled in different geometries and can be produced in 0, 1, 2, or 3 dimensions. The defining features of MOFs are their outstanding surface area, interconnected porosity, and variable chemical functionality, which enable an endless range of modalities for loading drugs into their hierarchical structures. MOFs, coupled with biocompatibility requisites, are now regarded as highly successful DDSs for the treatment of diverse diseases. This review aims to present the development and applications of DDSs based on chemically-functionalized MOF nanostructures in the context of cancer treatment. A concise overview of the structure, synthesis, and mode of action of MOF-DDS is provided. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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27 pages, 2947 KiB  
Review
The Properties of Microwave-Assisted Synthesis of Metal–Organic Frameworks and Their Applications
by Pham Thi Phan, Jeongsoo Hong, Ngo Tran and Thi Hoa Le
Nanomaterials 2023, 13(2), 352; https://doi.org/10.3390/nano13020352 - 15 Jan 2023
Cited by 29 | Viewed by 4040
Abstract
Metal–organic frameworks (MOF) are a class of porous materials with various functions based on their host-guest chemistry. Their selectivity, diffusion kinetics, and catalytic activity are influenced by their design and synthetic procedure. The synthesis of different MOFs has been of considerable interest during [...] Read more.
Metal–organic frameworks (MOF) are a class of porous materials with various functions based on their host-guest chemistry. Their selectivity, diffusion kinetics, and catalytic activity are influenced by their design and synthetic procedure. The synthesis of different MOFs has been of considerable interest during the past decade thanks to their various applications in the arena of sensors, catalysts, adsorption, and electronic devices. Among the different techniques for the synthesis of MOFs, such as the solvothermal, sonochemical, ionothermal, and mechanochemical processes, microwave-assisted synthesis has clinched a significant place in MOF synthesis. The main assets of microwave-assisted synthesis are the short reaction time, the fast rate of nucleation, and the modified properties of MOFs. The review encompasses the development of the microwave-assisted synthesis of MOFs, their properties, and their applications in various fields. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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15 pages, 2947 KiB  
Review
The Synthesis and Properties of TIPA-Dominated Porous Metal-Organic Frameworks
by Hongru Fu, Yuying Jiang, Fei Wang and Jian Zhang
Nanomaterials 2021, 11(11), 2791; https://doi.org/10.3390/nano11112791 - 21 Oct 2021
Cited by 3 | Viewed by 2018
Abstract
Metal-Organic Frameworks (MOFs) as a class of crystalline materials are constructed using metal nodes and organic spacers. Polydentate N-donor ligands play a mainstay-type role in the construction of metal−organic frameworks, especially cationic MOFs. Highly stable cationic MOFs with high porosity and open channels [...] Read more.
Metal-Organic Frameworks (MOFs) as a class of crystalline materials are constructed using metal nodes and organic spacers. Polydentate N-donor ligands play a mainstay-type role in the construction of metal−organic frameworks, especially cationic MOFs. Highly stable cationic MOFs with high porosity and open channels exhibit distinct advantages, they can act as a powerful ion exchange platform for the capture of toxic heavy-metal oxoanions through a Single-Crystal to Single-Crystal (SC-SC) pattern. Porous luminescent MOFs can act as nano-sized containers to encapsulate guest emitters and construct multi-emitter materials for chemical sensing. This feature article reviews the synthesis and application of porous Metal-Organic Frameworks based on tridentate ligand tris (4-(1H-imidazol-1-yl) phenyl) amine (TIPA) and focuses on design strategies for the synthesis of TIPA-dominated Metal-Organic Frameworks with high porosity and stability. The design strategies are integrated into four types: small organic molecule as auxiliaries, inorganic oxyanion as auxiliaries, small organic molecule as secondary linkers, and metal clusters as nodes. The applications of ratiometric sensing, the adsorption of oxyanions contaminants from water, and small molecule gas storage are summarized. We hope to provide experience and inspiration in the design and construction of highly porous MOFs base on polydentate N-donor ligands. Full article
(This article belongs to the Special Issue Advanced Metal-Organic Frameworks)
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