Solar-driven reforming of plastics offers a simple and low-energy means to turn waste into H₂. Here, we report the efficient photoreforming of three commonly produced polymers – polylactic acid, polyethylene terephthalate (PET) and polyurethane – using inexpensive CdS/CdO_x quantum dots in alkaline aqueous solution. This process operates under ambient temperature and pressure, generates pure H₂ and converts the waste polymer into organic products such as formate, acetate and pyruvate. We further validate the real-world applicability of the system by converting a PET water bottle into H₂. This is the first demonstration of visible light-driven, noble metal-free photoreforming of plastic.

Photocatalytic reforming of lignocellulosic biomass is an emerging approach to produce renewable H₂. This process combines photo‐oxidation of aqueous biomass with photocatalytic hydrogen evolution at ambient temperature and pressure. Biomass conversion is less energy demanding than water splitting and generates high‐purity H₂ without O₂ production. Direct photoreforming of raw, unprocessed biomass has the potential to provide affordable and clean energy from locally sourced materials and waste.

The development of high-performance electrocatalytic systems for the controlled reduction of CO₂ to value-added chemicals is a key goal in emerging renewable energy technologies. The lack of selective and scalable catalysts in aqueous solution currently hampers the implementation of such a process. Here, the assembly of a [MnBr(2,2′-bipyridine)(CO)₃] complex anchored to a carbon nanotube electrode via a pyrene unit is reported. Immobilization of the molecular catalyst allows electrocatalytic reduction of CO₂ under fully aqueous conditions with a catalytic onset overpotential of η = 360 mV, and controlled potential electrolysis generated more than 1000 turnovers at η = 550 mV. The product selectivity can be tuned by alteration of the catalyst loading on the nanotube surface. CO was observed as the main product at high catalyst loadings, whereas formate was the dominant CO₂ reduction product at low catalyst loadings. Using UV–vis and surface-sensitive IR spectroelectrochemical techniques, two different intermediates were identified as responsible for the change in selectivity of the heterogenized Mn catalyst. The formation of a dimeric Mn⁰ species at higher surface loading was shown to preferentially lead to CO formation, whereas at lower surface loading the electrochemical generation of a monomeric Mn-hydride is suggested to greatly enhance the production of formate. These results emphasize the advantages of integrating molecular catalysts onto electrode surfaces for enhancing catalytic activity while allowing excellent control and a deeper understanding of the catalytic mechanisms.