An investigation of two framework-based materials: novel phosphorus metal halides (M_xP_yX_z) and antimicrobial enabled [gamma]-CD-MOF-1

Gregory Schwenk

doi:10.17918/00001323

Although Phosphorus is perhaps one of the most well-known elements, a full understanding of its various allotropes and polymorphic subdivisions remains elusive. In concluding a general chemistry course, one may identify Phosphorus by three basic allotropes denoted by color: Red, White, and Black. However, owing to recent breakthroughs in nanomaterials, the allotropy of Phosphorus has broadened remarkably. Of these newly discovered forms, 1D nanorod structures, thought to be a derivative of Red Phosphorus polymorphs, are categorized by their resulting adduct character with metal halides. With a pure P nanorod surrounded by a metal interlayer and further encased by a halide layer, phosphorus metal halides (PMHs) have long been sought for their potential in identifying novel P nanorods that are stabilized within the structure. Furthermore, owing to their unique structure that combines the properties of a metal and a 1D phosphorus nanorod, they have recently seen an interest in electronic devices. To date, literature provides synthetic approaches that remain limited to CuI and CuBr with post-synthetic methods affording Ag₂P₃I₂, though with significant drawbacks. In this work, we establish synthetic routes to expand this family to include a novel Br-containing structure and establish Raman spectroscopy as a valid characterization method. Further, we have extended the family to incorporate the metals Ag and Pb in the form of Ag₃P₁₀I₂ and Pb₃P₁₅I₂. The synthetic approach that affords such structures is believed to be applicable to various transition metals via the in situ formation of MP_x, opening the door to extend the family of materials even further by introducing the MP_x as a precursor. Novel applications of devices constructed with Cu₂P₃I₂, Ag₂P₃I₂, Cu₂P₃Br₂, and Pb₃P₁₅I₂ have been established as molecular sensors and FETs. The optimization of synthetic conditions, particularly as it relates to Ag₃P₁₀I₂ has also revealed formation of large-scale Type II nanorods, a highly elusive polymorph of Red Phosphorus. Lastly, this work has encompassed another family of unique materials in the form of metal organic frameworks (MOFs). Herein, a particular variety of these porous materials, [gamma]-CD-MOF-1, has been shown capable of sequestration of benzalkonium chloride (BAC), a common disinfectant. By utilizing chemical vapor diffusion to grow the MOF on polypropylene fabric prior to BAC loading, we have developed a novel surfactant-impregnated MOF-coated fabric for antimicrobial applications. These surfactant-impregnated MOF-coated pieces of fabric were successful in displaying strong antibacterial character against Pseudomonas aeruginosa, Staphylococcus aureus, and Escherichia coli, as well as strong antiviral character against T4 bacteriophage and a murine betacoronavirus. All antibacterial and antiviral character was established and validated with comparison against controls.

An investigation of two framework-based materials: novel phosphorus metal halides (M_xP_yX_z) and antimicrobial enabled [gamma]-CD-MOF-1

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An investigation of two framework-based materials: novel phosphorus metal halides (M_xP_yX_z) and antimicrobial enabled [gamma]-CD-MOF-1

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