Chemoenzymatic Photoreforming: A Sustainable Approach for Solar Fuel Generation from Plastic Feedstocks.

Plastic upcycling through catalytic transformations is an attractive concept to valorize waste, but the clean and energy-efficient production of high-value products from plastics remains challenging. Here, we introduce chemoenzymatic photoreforming as a process coupling enzymatic pretreatment and solar-driven reforming of polyester plastics under mild temperatures and pH to produce clean H 2 and value-added chemicals. Chemoenzymatic photoreforming demonstrates versatility in upcycling polyester films and nanoplastics to produce H 2 at high yields reaching ∼10 3 -10 4 μmol g sub -1 and activities at >500 μmol g cat -1 h -1 . Enzyme-treated plastics were also used as electron donors for photocatalytic CO 2 -to-syngas conversion with a phosphonated cobalt bis(terpyridine) catalyst immobilized on TiO 2 nanoparticles (TiO 2 | CotpyP ). Finally, techno-economic analyses reveal that the chemoenzymatic photoreforming approach has the potential to drastically reduce H 2 production costs to levels comparable to market prices of H 2 produced from fossil fuels while maintaining low CO 2 -equivalent emissions.