This project aims to interrogate and design new methods for aerobic oxygenation of polyolefins (POs) to achieve two related goals: (1) prepare new polymeric materials with favorable properties and (2) convert mixed plastics waste into low molecular weight feedstock chemicals with high yield and selectivity. The upcycling and conversion of waste plastics within a circular carbon economy is a grand challenge. The major advantages of autoxidation methods include that it is thermodynamically favorable, resulting in significant energy savings and reduced CO2 footprint relative to pyrolysis, autoxidation- based PO depolymerization is compatible with mixed plastics, minimizing or avoiding the need for pre- sorting, it tolerates impurities, contaminants, and water, homogeneous autoxidation catalysts offer transport kinetic advantages over heterogeneous catalysts for polymer deconstruction and catalysts and initiators that support autoxidation are composed of robust, earth-abundant, recyclable materials.