Catalytic Methane Monofunctionalization by an Electrogenerated High-Valent Pd Intermediate
By O
Published in ACS Central Science
2017
Abstract
Electrophilic high-valent metal ions are potent intermediates for the catalytic functionalization of methane, but in many cases, their high redox potentials make these intermediates difficult or impossible to access using mild stoichiometric oxidants derived from O2. Herein, we establish electrochemical oxidation as a versatile new strategy for accessing high-valent methane monofunctionalization catalysts. We provide evidence for the electrochemical oxidation of simple PdSO4 in concentrated sulfuric acid electrolytes to generate a putative Pd2III,III species in an all-oxidic ligand field. This electrogenerated high-valent Pd complex rapidly activates methane with a low barrier of 25.9 (
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