Conversion of Polyethylene Waste into Gaseous Hydrocarbons via Integrated Tandem Chemical–Photo/Electrocatalytic Processes

[Image: see text] The chemical inertness of polyethylene makes chemical recycling challenging and motivates the development of new catalytic innovations to mitigate polymer waste. Current chemical recycling methods yield a complex mixture of liquid products, which is challenging to utilize in subsequent processes. Here, we present an oxidative depolymerization step utilizing diluted nitric acid to convert polyethylene into organic acids (40% organic acid yield), which can be coupled to a photo- or electrocatalytic decarboxylation reaction to produce hydrocarbons (individual hydrocarbon yields of 3 and 20%, respectively) with H(2) and CO(2) as gaseous byproducts. The integrated tandem process allows for the direct conversion of polyethylene into gaseous hydrocarbon products with an overall hydrocarbon yield of 1.0% for the oxidative/photocatalytic route and 7.6% for the oxidative/electrolytic route. The product selectivity is tunable with photocatalysis using TiO(2) or carbon nitride, yielding alkanes (ethane and propane), whereas electrocatalysis on carbon electrodes produces alkenes (ethylene and propylene). This two-step recycling process of plastics can use sunlight or renewable electricity to convert polyethylene into valuable, easily separable, gaseous platform chemicals.