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Development of Organic Linkers and Functionalized Metal Coordination Complexes: An Industrial Nose

Thesis Info

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Author

Mansab, Saira

Program

PhD

Institute

Fatima Jinnah Women University

City

Rawalpindi

Province

Punjab

Country

Pakistan

Thesis Completing Year

2019

Thesis Completion Status

Completed

Subject

Environmental Sciences

Language

English

Link

http://prr.hec.gov.pk/jspui/bitstream/123456789/12573/1/PhD%20thesis%20Red%20print.pdf

Added

2021-02-17 19:49:13

Modified

2024-03-24 20:25:49

ARI ID

1676724621769

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Currently, the scientists are directing their research in finding solutions for the risks associated with unanticipated and undetected chemical pollutants. The major efforts are focused on early identification and investigation of pollution issues before they worsen the environment and human health. In this aspect, new metal coordination complexes are explored as most sustainable materials. The efficiency can be tailor-made in terms of surface area, pore volume and conjugation of ligands for diverse sensing and remedial applications. The present research was aimed to synthesize single and mixed ligand coordination complexes based on nitrogen containing ligands (imidazole, triazole, pyridyl) with understanding that nitrogen has a significant role in binding with organic moiety. A series of coordination complexes were synthesized where both ligands were coordinated with zinc followed by post-synthesis modification for incorporation of amine groups. The assessment of structural surface and bulk properties was undertaken with a range of analytical techniques. Results of 1H-NMR identified structural modifications due to functionalization induced by amine moiety. The optimum (72% and 76%) incorporation was obtained for ethyl amine in imidazole and triazole, respectively. Further, binding of primary and secondary ligands in different ratios developed unique structures for mixed ligand coordination complexes. Another characteristic of complexes was binding of functional groups at amine position indicated by disappearance of distinctive (3000-3400cm-1) peak in FTIR analysis. The significance of the synthesized materials was their high structural and thermal stability due to metal coordination. However, incorporation of larger amine groups resulted in decrease in surface area. The synthesized single ligand and conjugated complexes were tested for adsorption and sensing potential against herbicide and nitro compounds, respectively. The highest (79%) adsorption efficiency was monitored for (Zn(NH-TBA)2Eth(NH2)2), due to maximum number of amine groups. The well-known adsorption isotherms and kinetics equation suggested that process pre-dominantly followed physio-sorption mechanism sequentially from sub-monolayer to multi-layered structure. Intra-particle model expressed three phase diffusion, via external surface, micropores and mesopores of the materials. The chemical sensing potential of conjugated (mixed ligand) complexes was determined through Photoluminescence studies. A blue shift with optimum intensity was recorded for complexes in comparison to ligand depicting the significant sensing for nitro compounds. Further, maximum quenching efficiency was noted for 4,4''- dibenzohydrazobenzene and nitroaniline, proposing collisional and static quenching mechanism. The electrical conductance of synthesized complexes was explored using impedance. An important aspect revealed was the charge transfer and diffusion resistance and radius of semicircle of Nyquist shifted to higher frequency due to increase in heterogeneity. These results were elaborated further by Randles-Ershler equivalent circuit model. The research submitted encouraging results opening a wide application window for the synthesized single-ligand and conjugated coordination complexes. The novelty of functionalization in complexes was also offered. The study testified the potential and efficacy as adsorbents, biosensors and semiconductors. The study concludes that these materials offer great capacity for commercial viability and suitable candidate for environmental remediation and luminescence-sensing applications.
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