ALKANE AND ARENE CH ACTIVATION WITH A THERMALLY, PROTIC AND OXIDANT STABLE IRIDIUM NNC PINCER COMPLEX

摘要

The CH Activation1 reaction could be utilized to develop the next generation of selective, hydrocarbon hydroxylation catalysts. Current CH Activation based systems that hydroxylate methane utilize "soft," redox-active electrophiles, such as Pd~(II), Pt~(IV), Hg~(II), Au~I. A key disadvantage of these systems is the requirement for strong acid solvents that leads to inhibition by Lewis basic products such as methanol. Indeed, while Pt(bpym)Cl2 efficiently hydroxylates methane in concentrated sulfuric acid, it is essentially inactive in CF3CO2H, HTFA. To overcome this, we are designing new generations of more electron-rich hydroxylation catalysts based on low to medium-valent metals to the left of Pt. Key challenges will be designing CH Activation catalysts that: A) are thermally stable to the protic, oxidizing conditions likely required and B) undergo facile Oxidative Functionalization of the CH Activation intermediates to generate the desired product.