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 similar to 10(3)-10(4) mu mol g(sub)(-1) and activities at >500 mu mol g(cat)(-1) h(-1). Enzyme-treated plastics were also used as electron donors for photocatalytic CO2-to-syngas conversion with a phosphonated cobalt bis(terpyridine) catalyst immobilized on TiO2 nanoparticles (TiO2|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 CO2-equivalent emissions.