Among the recent developments in metal-organic frameworks (MOFs), porous layered coordination polymers (CPs) have garnered attention due to their modular nature and tunable structures. These factors enable a number of properties and applications, including gas and guest sorption, storage and separation of gases and small molecules, catalysis, luminescence, sensing, magnetism, and energy storage and conversion. Among MOFs, two-dimensional (2D) compounds are also known as 2D CPs or 2D MOFs. Since the discovery of graphene in 2004, 2D materials have also been widely studied. Several 2D MOFs are suitable for exfoliation as ultrathin nanosheets similar to graphene and other 2D materials, making these layered structures useful and unique for various technological applications. Furthermore, these layered structures have fascinating topological networks and entanglements. This review provides an overview of different aspects of 2D MOF layered architectures such as topology, interpenetration, structural transformations, properties, and applications.

Two-Dimensional Metal-Organic Framework Materials: Synthesis, Structures, Properties and Applications.

This review analyzes the preparation and characterization of metal organic frameworks (MOFs) and their application as photocatalysts for water purification. The study begins by highlighting the problem of water scarcity and the different solutions for purification, including photocatalysis with semiconductors, such as MOFs. It also describes the different methodologies that can be used for the synthesis of MOFs, paying attention to the purification and activation steps. The characterization of MOFs and the different approaches that can be followed to learn the photocatalytic processes are also detailed. Finally, the work reviews literature focused on the degradation of contaminants from water using MOF-based photocatalysts under light irradiation.

https://www.mdpi.com/2073-4344/9/1/52/pdf

A Review on the Synthesis and Characterization of Metal Organic Frameworks for Photocatalytic Water Purification

Photoactive metal–organic frameworks (MOFs) have lately emerged as a class of crystalline porous materials, which provides an advanced platform to develop catalysts for the photocatalytic decolorization of wastewater. Controllable integration of pure MOFs into other active materials creates fabrication protocols for new multifunctional hybrids with superior photocatalytic properties for dye degradation into individual components, and the calcination of transition-metal MOF precursors affords a convenient and practical route for preparation of nanosized photocatalysts with novel structures and good purity. Although the application of pure MOFs for organic pollutant decomposition has been reviewed previously, there have been significant advances in diverse MOF-based composites and their derivatives for dye degradation, which have rarely been reviewed. This review aims to fill this gap and discuss the various influencing factors, the reaction kinetics, and mechanisms of dye degradation, considering the period from 2014 to 2016. Finally, the challenges and outlooks for dye decomposition by MOF-based materials are suggested.

Photocatalytic Decontamination of Wastewater Containing Organic Dyes by Metal–Organic Frameworks and their Derivatives

Various polyoxometalates (POMs) were successfully immobilized to the mesoporous coordination polymer MIL-101 resulting in a series of POM-MOF composite materials POM@MIL-101 (POM = K4PW11VO40, H3PW12O40, K4SiW12O40). These materials were synthesized by a simple one-pot reaction of Keggin POMs, tetramethylammonium hydroxide (TMAH), terephthalic acid (H2bdc), and Cr(3+) ions. XRD, FTIR, thermogravimetric analyses (TG), inductively coupled plasma (ICP) spectrometry, and energy-dispersive X-ray spectroscopy (EDX) collectively confirmed the successful combination of POMs and the porous framework. Further, these composites POM@MIL-101 with different loading of POMs were achieved by variation of the POM dosage. Notably, the uptake capacity of MIL-101 towards organic pollutants in aqueous solution was significantly improved by immobilization of hydrophilic POMs into cages of MIL-101. An uptake capacity of 371 mg g(-1), comparable to that of the graphene oxide sponges, and much higher than that of the commercial activated carbon, was achieved at room temperature in 5 min when dipping 20 mg PW11V@MIL-101 in the methylene blue (MB) solution (100 mL of 100 mg L(-1) MB solution). Further study revealed that the POM@MIL-101 composite materials not only exhibited a fast adsorption rate towards dye molecules, but also possessed of selective adsorption ability of the cationic dyes in wastewater. For example, the adsorption efficiency of PW11V@MIL-101 (10 mg) towards MB (100 mL of 10 mg L(-1)) could reach 98 % in the initial 5 min, and it could capture MB dye molecules from the binary mixture of the MB and MO with similar size. Also, the POM@MIL-101 materials could be readily recycled and reused, and no POM leached in the dye adsorption process.

Incorporating polyoxometalates into a porous MOF greatly improves its selective adsorption of cationic dyes.

To explore the influence of different aromatic polycarboxylates on the self-assembly and properties of d10 metal coordination frameworks, six coordination compounds containing a flexible bis(2-methylbenzimidazole) (pbmb) ligand, formulated as [Ag2(pbmb)(2,6-napdc)]n (1), {[Zn(pbmb)(tbta)]·H2O}n (2), {[Cd(pbmb)(tbta)]·H2O}n (3), [Zn2(pbmb)(btec)(H2O)]n (4), {[Zn2(OH)(pbmb)(bpdc)1.5]·H2O}n (5), and [Cd(pbmb)(3-npa)(H2O)]n (6), have been synthesized under hydrothermal conditions and characterized by physicochemical and spectroscopic methods as well as single-crystal X-ray diffraction analysis (2,6-H2napdc = 2,6-naphthalenedicarboxylic acid, H2tbta = tetrabromoterephthalic acid, H4btec = 1,2,4,5-benzenetetracarboxylic acid, H2bpdc = biphenyl-4,4′-dicarboxylic acid and H23-npa = 3-nitrophthalic acid). Complex 1 possesses an 8-connected 3D coordination framework with sqc3 topology based on rare tetranuclear Ag(I)-cluster secondary building units (SBUs). 2 and 3 possess 2D (4,4) grid structures. 4 shows a novel (3,4,5)-connected 2D network with the Schlafli symbol of {3·4·5}{3·42·52·6}{3·43·53·6·72}. 5 features a uninodal (4,4)-connected net containing binuclear {Zn2(OH)} SBUs and a 2-fold interpenetrating (3,6)-connected supramolecular framework with {42·6}{44·610·8}-3,6T24 topology that is formed via hydrogen bond interactions. Complex 6 is a 1D double-chain structure, which is finally extended to a 3D (4,5,5)-connected supramolecular network via hydrogen bonding interactions. Complexes 1–6 indicate high thermal stabilities and different photoluminescence behavior in the solid state. Moreover, all of these polymer materials manifest excellent photocatalytic activities for the degradation of methyl orange in the photo-Fenton-like process after 120 min (1: 99%, 2: 66%, 3: 91%, 4: 83%, 5: 91% and 6: 93%, respectively).

A series of d10 metal coordination polymers based on a flexible bis(2-methylbenzimidazole) ligand and different carboxylates: synthesis, structures, photoluminescence and catalytic properties

To systematically explore the effect of polynuclear complexes on photocatalytic degradation of the organic dyes, a series of coordination complexes containing CdII clusters, formulated as {[Cd3L2(H2O)5]·H2O}n (1), {[Cd3L2(hbmb)(H2O)2]·2.5H2O}n (2), {[Cd3L2(btbb)(H2O)2]·2EtOH·1.5H2O}n (3), and {[Cd6L4(bipy)2(H2O)6]·3H2O}n (4) (H3L = 3,4-bi(4-carboxyphenyl)-benzoic acid, hbmb = 1,1′-(1,6-hexane)bis(2-methylbenzimidazole), btbb = 1,4-bis(2-(4-thiazolyl)benzimidazole-1-ylmethyl)benzene, 4,4′-bipy = 4,4′-bipyridine), have been designed and synthesized. Complex 1 based on trinuclear CdII clusters exhibits a new (3,3,6)-connected 3D framework. 2 belongs to a (3,3,8,8)-connected tfz-d topology net with pillar-layered frameworks assembled by two kinds of trinuclear CdII clusters. 3 is a 3D pillar-layered framework, which features a (3,8)-connected tfz-d net based upon one kind of trinuclear CdII cluster. 4 presents a new 3D (3,6,10)-connected framework with dinuclear and tetranuclear clusters. The photocatalytic p...

Polynuclear CdII Polymers: Crystal Structures, Topologies, and the Photodegradation for Organic Dye Contaminants

Tuned by different aromatic polycarboxylates, six fascinating coordination polymers (CPs), namely, [Cd(pbmb)(p-bdc)]n (1), {[Zn3(pbmb)2(1,3,5-btc)2]·6H2O}n (2), {[Cd3(pbmb)3(1,3,5-btc)2(H2O)]·3H2O}n (3), {[Zn2(pbmb)(1,2,3-btc)(μ2-OH)]·H2O}n (4), [Cd(pbmb)(1,2,4,5-btec)0.5]n (5), and {[Cd(pbmb)(sdba)]·2H2O}n (6) (pbmb = 1,1′-(1,3-propane)bis-(2-methylbenzimidazole), p-H2bdc = 1,4-benzenedicarboxylic acid, 1,3,5-H3btc = 1,3,5-benzenetricarboxylic acid, 1,2,3-H3btc = 1,2,3 benzenetricarboxylic acid, 1,2,4,5-H4btec = 1,2,4,5-benzenetetracarboxylic acid, H2sdba = 4,4′-sulfonyldibenzoic acid), have been ideated and synthesized by hydrothermal reaction methods. Structural analyses reveal that complexes 1–3 feature three-dimensional (3D) structures (1: 4-connected 66 topology, 2: (3,4,6)-connected (65·7)(4·62)2(42·66·85·102) topology and 3: (2,3,4)-connected (65·8)2(63)2 topology), and the remaining CPs 4–6 exhibit 2D networks. The thermal stability and powder X-ray diffraction for 1–6 have been investigated as further properties. The optical band gaps are analyzed by diffuse-reflectance UV-vis spectra. Moreover, all of the materials manifest good photocatalytic activities for the degradation of methylene blue (MB) (1: 74%, 2: 41%, 3: 37%, 4: 76%, 5: 46%, 6: 75%, respectively) in water under the irradiation of a high-pressure mercury lamp.

Novel coordination polymers of Zn(II) and Cd(II) tuned by different aromatic polycarboxylates: synthesis, structures and photocatalytic properties

A series of novel CdII coordination complexes, formulated as {[Cd(btbb)0.5(p-phda)]·H2O}n (1), [Cd(btbb)0.5(oba)]n (2), {[Cd2(btbb)(m-bdc)2(H2O)]·2H2O}n (3), {[Cd(btbb)0.5(btec)0.5(H2O)]·2H2O}n (4), [Cd(btbb)0.5(o-bdc)]n (5) and {[Cd2(btbb)(bptc)(H2O)]·4H2O}n (6) (btbb = 1,4-bis(2-(4-thiazolyl)benzimidazol-1-ylmethyl)benzene, H2phda = phenylenediacetic acid, H2oba = 4,4′-oxybis(benzoic acid), m-H2bdc = 1,3-benzenedicarboxylic acid, H4btec = 1,2,4,5-benzenetetracarboxylate, o-H2bdc = 1,2-benzenedicarboxylic acid, H4bptc = 3,3′,4,4′-benzophenone tetracarboxylic acid), have been obtained by solvothermal/hydrothermal reactions for the exploration of efficient photocatalytic degradation of organic dye pollutants. Complex 1 features a 6-connected 3D pcu α-Po primitive cubic topology net with the point symbol 412·63. Interestingly, complexes 2, 3 and 5 contain left- and right-handed helical chains (2: a 2-fold interpenetrating 3D architecture with {412·63}-pcu topology network; 3: a (3,6)-connected net with a vertex symbol (42·54·66·7·82)(4·62); 5: a (3,4)-connected 3,4L83 topology net with point symbol (42·6)(42·63·8)). Complex 4 exhibits a (3,4)-connected 3,4T48 topology net with point symbol (84·102)(8·102), while complex 6 possesses a (3,5)-connected 3,5L2 topology with the point symbol (42·6)(42·67·8). Furthermore, the photophysical studies indicate that the relatively narrow optical energy gaps of complexes 1–6 (<2.30 eV) calculated from the diffuse reflectivity spectra reflect their outstanding semiconductive nature. The photocatalytic properties of complexes 1–6 were studied in detail, and the results demonstrate their good photocatalytic activities in methylene blue (MB) degradation reactions, especially for complexes 3, 4 and 6 (3: 91.4%, 4: 92.7%, 6: 86.7%).

Structural variability, topological analysis and photocatalytic properties of neoteric Cd(II) coordination polymers based on semirigid bis(thiazolylbenzimidazole) and different types of carboxylic acid linkers

To seek the effect that condition of the complexes has on the manufacture of the biaryl compounds, seven Ni(II) complexes, namely, {[Ni(L)0.5(bpa)(H2O)]·2H2O}n (1), {[Ni2(L)(dpp)2(H2O)]·4H2O}n (2), {[Ni(L)0.5(pbmb)(H2O)]·H2O}n (3), {[Ni2(L)(bmp)2(H2O)]·7H2O}n (4), {[Ni(L)0.5(pbib)1.5]·2H2O}n (5), {[Ni2(L)(pbib)1.5]·3H2O}n (6), and [Ni(L)0.5(beb)2(H2O)]n (7) (bpa = 1,2-bis(4-pyridyl)ethane, dpp = 1,3-di(4-pyridyl)propane, pbmb = 1,1′-(1,3-propane)bis(2-methylbenzimidazole), bmp = 1,5-bis(2-methylbenzimidazol) pentane, pbib = 1,4-bis(imidazol-1-ylmethyl)benzene, beb = 1,4-bis(2-ethylbenzimidazol-1-ylmethyl)benzene), have been gained through hydro(solvo)thermal reactions of 5,5′-(hexane-1,6-diyl)-bis(oxy)diisophthalic acid ligand (H4L) with Ni(II) metal ions under the regulation and control of six N-donor ligands. 3-fold interpenetrating complex 1 belongs to a (4,4)-connected 3D bbf net with a vertex symbol of (64·82)(66) topology. 3-fold interpenetrating complex 2 presents a (4,4,4)-connected 3D bbf net wit...

Ni(II) Coordination Polymers Constructed from the Flexible Tetracarboxylic Acid and Different N-Donor Ligands: Structural Diversity and Catalytic Activity

To explore new 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (BODIPY)-derived metal–organic frameworks (MOFs), we employed 2,6-dicarboxyl-1,3,5,7-tetramethyl-8-phenyl-4,4-difluoroboradiazaindacene (H2L) as a ligand to successfully synthesize five coordination polymers, namely, {[Zn2(L)2(bpp)]·2H2O·2EtOH}n (1), {[Cd2(L)2(bpp)]·2H2O·EtOH}n (2), {[Cd2(L)(bpe)3(NO3)2]·2H2O·DMF·EtOH}n (3), {[Cd(L)(bpe)0.5(DMF)(H2O)]}n (4), and {[Cd(L)(bpe)0.5]·1.5H2O·DMF}n (5) (bpp = 1,3-bi(4-pyridyl)propane, bpe = 1,2-bi(4-pyridyl)ethane). Except for two 2D-layer coordination polymers 3 and 4, the rest samples exhibit 3D metal–organic frameworks with certain pore sizes, especially MOFs 1 and 5. Spectroscopic and crystallographic investigations demonstrate that the absorption and emission energies of the BODIPY chromophores are sensitive to the coordination modes. Moreover, in case 2, the transition metal centers coordinated with the dicarboxylate ligands L2– are capable of forming the two BODIPY units in coplanar arrangements (θ...

Spectroscopic and Crystallographic Investigations of Novel BODIPY-Derived Metal–Organic Frameworks

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