Synthesis of mixed ligand and pillared paddlewheel MOFs using waste polyethylene terephthalate material as sustainable ligand source

Conjugated alkali metal dicarboxylates have recently received attention for applications as organic anode materials in lithium-and sodium-ion batteries.In order to understand and optimise these materials, it is important to be able to characterise both the long-range and local aspects of the crystal structure, which may change during battery cycling. Furthermore, some materials can display polymorphism or hydration behaviour. NMR crystallography, which combines long-range crystallographic information from diffraction with local information from solid-state NMR via interpretation aided by DFT calculations, is one such approach, but this has not yet been widely applied to conjugated dicarboxylates. In this work, we evaluate the application of NMR crystallography for a set of model lithium and sodium dicarboxylate salts. We investigate the effect of different DFT geometry optimisation strategies and find that the calculated NMR parameters are not systematically affected by the choice of optimisation method, although the inclusion of dispersion correction schemes is important to accurately reproduce the experimental unit cell parameters. We also observe hydration behaviour for two of the sodium salts and provide insight into the structure of an as-yet uncharacterised structure of sodium naphthalenedicarboxylate. This highlights the importance of sample preparation and characterisation for organic sodium-ion battery anode materials in particular.

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“…In principle, these organic coordination polymers can be derived from green and sustainable sources or from recycled waste plastic. [ 1,2 ]…”

Section: Introductionmentioning

confidence: 99%

A structural investigation of organic battery anode materials by NMR crystallography

Seymour

Griffiths

Halcovitch

et al. 2022

Magnetic Reson in Chemistry

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“…HCl, DMF, and DABCO were mixed and heated to 100–120 °C for 48 h. All the MOFs were obtained in 90–95% yield. 111 Similarly, Lo et al synthesized a series of nanoporous MOFs such as MIL (47, 53, and 101) using polyethylene terephthalate (PET) plastic-derived organic linkers. Furthermore, besides MIL-47 (V), other MOFs were formed as an amorphous powder.…”

Section: Metal–organic Framework (Mofs)mentioning

confidence: 99%

Metal–organic frameworks (MOFs) for energy production and gaseous fuel and electrochemical energy storage applications

Shanmugam,

Agamendran,

Sekar

et al. 2023

Phys. Chem. Chem. Phys.

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“…Mixed-ligand MOFs, namely [M 2 (BDC) 2 (DABCO)], where M = Fe(II), Co(II), Ni(II), Cu(II) and Zn(II); and DABCO = 1,4- diazabicyclo[2.2.2]octane), have been prepared in a one-pot reaction by employing PET waste as BDC source in presence of an inorganic acid to facilitate PET depolymerization [ 141 ], demonstrating that the topology of the PET-derived MOFs can be further tuned and expanded by adding other different organic ligands during the synthesis procedure.…”

Section: Plastic Waste As Linker Source For Mofs Adsorbentsmentioning

confidence: 99%

Metal-organic frameworks and plastic: an emerging synergic partnership

Mastropietro

2023

Science and Technology of Advanced Materials

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Mismanagement of plastic waste results in its ubiquitous presence in the environment. Despite being durable and persistent materials, plastics are reduced by weathering phenomena into debris with a particle size down to nanometers. The fate and ecotoxicological effects of these solid micropollutants are not fully understood yet, but they are raising increasing concerns for the environment and people’s health. Even if different current technologies have the potential to remove plastic particles, the efficiency of these processes is modest, especially for nanoparticles. Metal-organic frameworks (MOFs) are crystalline nano-porous materials with unique properties, have unique properties, such as strong coordination bonds, large and robustus porous structures, high accessible surface areas and adsorption capacity, which make them suitable adsorbent materials for micropollutants. This review examines the preliminary results reported in literature indicating that MOFs are promising adsorbents for the removal of plastic particles from water, especially when MOFs are integrated in porous composite materials or membranes, where they are able to assure high removal efficiency, superior water flux and antifouling properties, even in the presence of other dissolved co-pollutants. Moreover, a recent trend for the alternative preparation of MOFs starting from plastic waste, especially polyethylene terephthalate, as a sustainable source of organic linkers is also reviewed, as it represents a promising route for mitigating the impact of the costs deriving from the widescale MOFs production and application. This connubial between MOFs and plastic has the potential to contribute at implementing a more effective waste management and the circular economy principles in the polymer life cycle.

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Synthesis of mixed ligand and pillared paddlewheel MOFs using waste polyethylene terephthalate material as sustainable ligand source

Cited by 20 publications

References 34 publications

A structural investigation of organic battery anode materials by NMR crystallography

A structural investigation of organic battery anode materials by NMR crystallography

Metal–organic frameworks (MOFs) for energy production and gaseous fuel and electrochemical energy storage applications

Metal-organic frameworks and plastic: an emerging synergic partnership

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