Oxygen vacancy mediated oxidative reforming of polylactic acid to hydrocarbon

Degradable plastic, while attractive, pose environmental risks due to easy microplastics production. This study targets converting degradable plastics into high-value chemicals to address plastic pollution and resource utilization. Improving product selectivity during oxide species-modulated plastic conversion remains challenging in Fenton-like processes. We propose a singlet oxygen ( 1 O 2 )-driven strategy for selective polylactic acid (PLA) conversion to hydrocarbons. Peroxymonosulfate (PMS) is activated by Cu-Mg co-doped 3D nickel sulfides with oxygen vacancies . More vacancies lower the O-O bond breakage energy in PMS and enhance 1 O 2 generation. As designed, C α -O sites of PLA are electrophilicly attacked by 1 O 2 . 1 O 2 provides suitable energy for hydrogen extraction from tertiary C α -H and methyl C-H, generating vital R-COO • and R • . Hydrocarbons are formed after CO 2 removal from R-COO • . 1 O 2 -initiated radicals generation overcomes key barriers in PLA conversion. Impressively, Techno-economic analysis (TEA) and life cycle assessment (LCA) suggest that the process can effectively reduce carbon emissions and provide favorable economic benefits. This hydrothermal oxidation process is expected to solve the issues of environmental pollution and carbon waste caused by PLA. The present development has great potential for recycling of carbon resources with a negligible environmental footprint. • Oxygen vacancies promote O-O bond breaking in PMS and 1O2 generation. • 1O2 attacks the Cα-O sites of PLA electrophilically to realize depolymerization. • PLA was directionally converted into hydrocarbons via vital R-COO• and R•. • High-value conversion PLA reduces carbon emissions and increases economic benefits.