Design, Synthesis and Spectroscopic Characterization of Iron Based Molecular Catalysts for Water Oxidation

Halder, Jyotirmoy and Maji, Somnath (2018) Design, Synthesis and Spectroscopic Characterization of Iron Based Molecular Catalysts for Water Oxidation. Masters thesis, Indian Institute of Technology Hyderabad.

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Abstract

The continuous increase in global energy consumption leads to find an alternative source of carbon-based fuel. One of the promising solutions is the artificial photosynthesis which follows a different mechanistic pathway than that of the natural photosynthesis in the green plant, but the fundamental principles remain the same, i.e., to reserve the solar energy in the form of chemical energy. Water oxidation is the promising and sustainable solution for that purpose. But the splitting of water requires a molecular catalyst, and in this thesis, the synthesis of iron-based molecular catalysts as Water Oxidation Catalyst (WOC) will be discussed. Molecular catalysts for the water oxidation are generally comprised of a good ligand framework, i.e., polypyridyl system or nitrogen-containing aromatic or chelating compounds. After a thorough mechanistic studies of the literature, it has been observed that negatively charged ligand system in the WOCs are better choices as they can decrease the redox potential of metal complexes. Here a series of anionic ligands and their metal complexes have been synthesized and successfully characterized by different spectroscopic tools such as NMR, FTIR, and ESI-HRMS. The synthesized ligands are 2-Pyridinecarboxamide, N-(4-methylphenyl) (L1); 2-Pyridinecarboxamide, N-(4-bromophenyl) (L2); 2-Pyridinecarboxamide, N-8 quinolinyl (L3); N, N’-1, 4-Phenylenebis [2-pyridinecarboxamide] (L4); and the metal complex [Fe(pcq)(bpy)Cl]Cl (M1)which will be tested as potential water oxidation catalyst and mechanistic study will be also performed. Efforts to grow suitable single crystals for our synthesized ligands as well as metal complexes also attempted.

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