Interfacial W–O–Zr ensembles in tungstated zirconia catalysts enable efficient hydrogen-free recycling of polypropylene waste

Polyolefins are essential plastics to modern life yet create mounting sustainability challenges. Chemical recycling technologies are key but often require harsh conditions, costly hydrogen, noble metals, or complex catalysts with challenging design. We report hydrogen- and solvent-free depolymerization of polypropylene consumer goods at 240 °C, achieving >80% yield into gasoline hydrocarbons with stable performance. A library of tungstated zirconia catalysts synthesized by flame spray pyrolysis with controlled tungsten speciation enables correlating performance with the density of W-O-Zr ensembles prevalent in sub-nanoclusters, with W:Zr = 1:9 emerging as optimal. These acid sites formed during reaction mediate internal hydrogen transfer and selective backbone C-C scission, as deduced from operando spectroscopy. Life cycle and technoeconomic studies, benchmarked against hydrotreatment-based recycling in a harmonized framework, indicate competitive environmental and economic advantages. Together, this work establishes this route's promise and underscores the value of precision catalyst synthesis in polyolefin valorization.