Non-equilibrium plasma co-upcycling of waste plastics and CO2 for carbon-negative oleochemicals†

Mechanical recycling and chemical upcycling by thermochemical reactions have been the major approaches for recycling end-of-life plastics. Herein, we report an electrified approach to upcycle waste plastics into carbon-negative commodity chemicals using greenhouse gas CO₂ as the oxidant and additional carbon source. In this non-equilibrium plasma process, waste polyolefins were oxidatively depolymerized by plasma-activated CO₂ to produce oleochemicals and hydrocarbon chemicals in a single-step process at high reaction rates. In addition, a mixture of CO₂ and a small amount of O₂ was employed as plasma gases to selectively produce fatty alcohols from polyolefins. Based on this atmospheric pressure, non-solvent, and non-catalyst process, up to 97.6% of fatty alcohols could be produced within minutes. In this article, the co-conversion approach was demonstrated using common polyolefins and real-world mixed waste plastics to obtain comparable results. The techno-economic analysis estimates the internal rate of return to be 42.2% and 43.5% for the plasma-based conversion of waste plastics, depending on the plasma gas composition. Lifecycle assessment indicates the global warming potential is between −3.33 and −3.07 kg CO_2e per kg of plastic.