Executive Summary : | Late-stage selective functionalization of organic molecules via C-H bond activation is crucial for pharmaceutical and materials industries, as most fine chemicals and drug molecules are derived from natural feedstock of oil and hydrocarbons through multistep synthesis. However, activating strong C-H bonds in hydrocarbons is often challenging due to their strong nature. Large-scale oxygenation of hydrocarbons is typically achieved through combustion in the presence of oxygen and reaction with superacid, leading to non-selective oxygenation and overoxidation to carbon dioxide. Nature has evolved with bio-catalysts (metalloenzymes) capable of selective and efficient C-H functionalization under ambient reaction conditions. A large family of oxygenases and halogenases facilitate selective hydroxylation and halogenation via a two-step mechanism of hydrogen atom transfer followed by hetero-atom transfer. However, the large scale practical feasibility of these metalloenzymes is hampered by their low stability and productivity. synthetic complexes have been designed to mimic the structure, electronic properties, and reactivity of native enzymes. However, most halogenase model complexes suffer from competitive hydroxylation. In my postdoctoral work, we have shown that high-valent metal-halides are competent HAT entities and can selectively fluorinate saturated hydrocarbons without forming oxygenated products. In my independent research career, I envision exploring the synthesis and reactivity studies on high-valent metal-nitrido-halide complexes as potential C-H bond activators. |