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Hybrid MOFs for Catalytic Applications

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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (15 October 2022) | Viewed by 16917

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Prof. Dr. Rafael Luque

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Departamento de Química Orgánica, Universidad de Córdoba, Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km 396, Córdoba, Spain
Interests: green chemistry; biomass valorization; heterogeneous catalysis; nanomaterial design
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Dr. Francisco G. Cirujano

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Instituto de Ciencia Molecular (ICMol), Universitat de València, Catedrático José Beltrán Martínez nº 2, 46980 Paterna, Valencia, Spain
Interests: confined catalysis; organic synthesis; reticular chemistry; ordered porous hybrid organic–inorganic solids; fine chemicals, active pharmaceutical ingredients

Prof. Dr. Amarajothi Dhakshinamoorthy

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School of Chemistry, Madurai Kamaraj University, Madurai 625 021, India
Interests: heterogeneous catalysis; metal–organic frameworks; solid catalysts; chitosan; carbocatalysis
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Special Issue Information

Dear Colleagues,

The catalytic applications of metal–organic frameworks (MOFs) have been growing exponentialy in recent years due to their excellent characteristics of high porosity, chemical versatility, and tailorable design of catalytic active sites. In order to improve mechanical, thermal or chemical stability under reaction conditions, the development of hybrid forms of MOFs with other materials, such as silicoaluminates, carbon, polymers, nanoparticles, etc., is growing extremely fast, given the improved properties compared to those of bulk parent MOFs. Therefore, a compilation of the latest advances in the field would be useful to connect interested authors and readers. This Special Issue aims to cover recent and emerging strategies for the synthesis and catalytic applications of MOF hybrid materials, focusing on the aspects that drive present and future research, from synthesis of hybrid materials to their applications in chemical, environmental or energy-related catalysis or other surface or confined chemistry phenomena involving relevant chemical transformations of value-added molecules. For authors, this issue will be a good opportunity to publish their original research after peer review by expert researchers of hybrid porous solids and catalysis for a sustainable chemistry. Review articles by experts in such fields of research are also strongly encouraged to be submitted for publication in this Special Issue.

Prof. Dr. Rafael Luque
Dr. Francisco G Cirujano
Prof. Amarajothi Dhakshinamoorthy
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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Keywords

Metal–organic frameworks (MOFs)
Hybrid organic–inorganic materials
Hierarchical materials
Coordination polymers
Mesoporous (organo)silica
Covalent organic framework
Heterogeneous catalysis
Adsorption–separation phemomena
Supramolecular/host–guest chemistry

Published Papers (7 papers)

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Research

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12 pages, 5354 KiB

Open AccessArticle

NH₂-Modified UiO-66: Structural Characteristics and Functional Properties

by Konstantin L. Timofeev, Sergei A. Kulinich and Tamara S. Kharlamova

Molecules 2023, 28(9), 3916; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules28093916 - 05 May 2023

Cited by 6 | Viewed by 2676

Abstract

The development of new functional materials based on metal–organic frameworks (MOFs) for adsorption and catalytic applications is one of the promising trends of modern materials science. The Zr-based MOFs, specifically UiO-66, are considered as the supports for metallic catalysts for the 5-hydroxymethylfurfural platform molecule reduction into valuable products. The present work focused on the effect of NH₂ modification of UiO-66 on its structure and functional properties. The samples were prepared by a solvothermal method. The structure of the obtained materials was studied by X-ray diffraction, IR spectroscopy, UV–visible spectroscopy, and low-temperature nitrogen adsorption. Basic properties were investigated by HCl and CH₃COOH adsorption, and electrokinetic properties were studied by electrophoretic light scattering. UiO-66-NH₂ samples with different contents of aminoterephthalate linkers were successfully prepared. A gradual decrease in the specific surface area and the fraction of micropores with a diameter of ~0.9 nm was observed with an increase in the aminoterephthalate content. A proportional increase in the total number of basic sites in UiO-66-NH₂ samples was established with an increase in the aminoterephthalate content up to 75%. At the same time, a noticeable decrease in the total number of basic sites and an increase in their strength with higher aminoterephthalate content was observed. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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0 pages, 1627 KiB

Open AccessFeature PaperArticle

Carbazole and Diketopyrrolopyrrole-Based D-A π-Conjugated Oligomers Accessed via Direct C–H Arylation for Opto-Electronic Property and Performance Study

by Xiaofeng Zhang, Lingwei Feng, Kai Zhang and Shi-Yong Liu

Molecules 2022, 27(24), 9031; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27249031 (registering DOI) - 18 Dec 2022

Cited by 5 | Viewed by 1943

Abstract

Five carbazole and diketopyrrolopyrrole-based donor-acceptor (D-A) new π-conjugated oligomers (π-COs) with gradually elongated lengths are facilely synthesized via a single pot of direct C–H arylation with merits of atom- and step-economy. The structure-property-performance correlations of these π-COs and their parent polymer are studied in detail by opto-electronic characterizations and bulk heterojunction (BHJ) organic photovoltaic (OPV) devices. It is found that the π-COs having longer lengths enable better performance in OPVs owing to the enhanced intermolecular interaction with the elongation of the conjugations. The above results not only highlight the powerful synthetic strategy here provided, but also reveal that π-COs with unique properties might find promising application in OPVs. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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9 pages, 1533 KiB

Open AccessArticle

Dinuclear Lanthanide Compound as a Promising Luminescent Probe for Al³⁺ Ions

by Zhi Chen, Yinghao Xie, Zhanbo Li and Tao Lin

Molecules 2022, 27(24), 8761; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27248761 - 10 Dec 2022

Cited by 2 | Viewed by 1139

Abstract

Luminescent probes have wide applications in biological system analysis and environmental science. Here, one novel luminescent dinuclear europium compound with a crown ether analogous ligand was synthesized through a solvent–thermal reaction. Through transformation, upon the addition of Al³⁺ ions to the N,N′-dimethyl formamide solution of the europium compound, the luminescent intensity of the characteristic emission of Eu³⁺ decreased, and a new emission peak appeared at 346 nm and increased rapidly. The luminescent investigation indicated that it could act as a highly sensitive and selective luminescent probe for Al³⁺ ions. Moreover, mass spectrometry and single-crystal X-ray diffraction confirmed the formation of a new more stable trinuclear aluminium compound during the sensing process. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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15 pages, 4517 KiB

Open AccessFeature PaperArticle

Fast Assembly of Metal Organic Framework UiO-66 in Acid-Base Tunable Deep Eutectic Solvent for the Acetalization of Benzaldehyde and Methanol

by Lifang Chen, Xiangzhu Ye, Ting Zhang, Hao Qin, Hongye Cheng and Zhiwen Qi

Molecules 2022, 27(21), 7246; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27217246 - 25 Oct 2022

Cited by 3 | Viewed by 2002

Abstract

Zirconium-based metal-organic frameworks (MOFs) have attracted extensive attention owing to their robust stability and facile functionalization. However, they are generally prepared in common volatile solvents within a long reaction time. Here, we introduced environmentally friendly, cheap, and acid-based tunable deep eutectic solvents (DESs) formed from 2-methyl imidazole (MIm) and p-toluenesulfonic acid (PTSA) which significantly accelerated the assembly of zirconium-based MOF (UiO-66) without any aggressive additives. PTSA in acidic DES and ZrOCl₂ preliminarily formed Zr(IV) oxo organic acid framework, whereas basic DES completely dissolved the ligand of UiO-66. The strong hydrogen bond effect of PTSA and MIm efficiently accelerated the linker exchange between zirconium oxo organic coordination in acidic DES and benzenedicarboxylate linker in weak basic DES within a reaction time of 2 h at 50 °C. Thus, UiO-66 was quickly assembled with small particle sizes and used as an excellent catalyst for the acetalization of benzaldehyde and methanol. Therefore, the developed synthesis approach provides a new green strategy to quickly prepare and design various structures of metal-based compounds under mild reaction conditions. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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10 pages, 1548 KiB

Open AccessArticle

MOF-808 as a Highly Active Catalyst for the Diastereoselective Reduction of Substituted Cyclohexanones

by Hans Hilmar Mautschke and Francesc X. Llabrés i Xamena

Molecules 2022, 27(19), 6315; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules27196315 - 25 Sep 2022

Cited by 2 | Viewed by 1526

Abstract

Zr-containing MOF-808 is an excellent heterogeneous catalyst for the diastereoselective Meerwein–Ponndorf–Verley reduction of substituted cyclohexanones. The presence of substituents at the 2 or 3 position of the cyclohexanone ring strongly drives the reaction towards the formation of one of the two possible isomers. For 3-methyl cyclohexanone, the available space inside the MOF pores allows the formation of the bulkier transition state leading to the thermodynamically stable 3-cis-cyclohexanol. For 2-methyl cyclohexanone, the reaction rate is much slower and the final diastereoselectivity depends on the size of the alcohol used. Finally, reduction of 2-phenyl cyclohexanone is considerable faster over MOF-808 than for any other catalyst reported so far. The large size of the phenyl favors the selective formation (up to 94% selectivity) of the cis-alcohol, which goes through a less hindered transition state. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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18 pages, 3852 KiB

Open AccessArticle

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO₂ with Tunable Missing-Linker Defects

by Chunhua Wang, Zhiquan Yu, Yuhao Yang, Zhichao Sun, Yao Wang, Chuan Shi, Ying-Ya Liu, Anjie Wang, Karen Leus and Pascal Van Der Voort

Molecules 2021, 26(19), 5736; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26195736 - 22 Sep 2021

Cited by 12 | Viewed by 2868

Abstract

Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO₂, by impregnation using a double-solvent method (DSM) followed by H₂ reduction. The obtained Pd/UiO-66-NO₂ catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO₂ exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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Review

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16 pages, 2341 KiB

Open AccessReview

Metal-Organic Frameworks as Versatile Heterogeneous Solid Catalysts for Henry Reactions

by Francisco G. Cirujano, Rafael Luque and Amarajothi Dhakshinamoorthy

Molecules 2021, 26(5), 1445; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26051445 - 07 Mar 2021

Cited by 30 | Viewed by 3557

Abstract

Metal–organic frameworks (MOFs) have become one of the versatile solid materials used for a wide range of applications, such as gas storage, gas separation, proton conductivity, sensors and catalysis. Among these fields, one of the more well-studied areas is the use of MOFs as heterogeneous catalysts for a broad range of organic reactions. In the present review, the employment of MOFs as solid catalysts for the Henry reaction is discussed, and the available literature data from the last decade are grouped. The review is organized with a brief introduction of the importance of Henry reactions and structural properties of MOFs that are suitable for catalysis. The second part of the review discusses the use of MOFs as solid catalysts for the Henry reaction involving metal nodes as active sites, while the third section provides data utilizing basic sites (primary amine, secondary amine, amides and urea-donating sites). While commenting on the catalytic results in these two sections, the advantage of MOFs over other solid catalysts is compared in terms of activity by providing turnover number (TON) values and the structural stability of MOFs during the course of the reaction. The final section provides our views on further directions in this field. Full article

(This article belongs to the Special Issue Hybrid MOFs for Catalytic Applications)

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