7 billion of 9.2 billion tons of plastic produced becomes waste while conventional catalytic plastic recycling methods are vulnerable with degraded performance and intensive energy input. Here, a hybrid Zn/b-ZnO catalyst, together with the specially-designed microwave reaction system, has achieved fast plastic waste upgrading under atmospheric pressure without using H2. Bifunctional ZnO acts as a microwave absorber and substrate catalyst, and in-situ formed Zn clusters promote C-C bond cleavage and nearly 100% upcycle landfilled plastic mixtures into lubricant base oil precursors and monomers. Unprecedented turnover number (250 gplastic g−1catalyst) of plastic depolymerisation and long-time stability over 50 successive cycles have been demonstrated, together with 8-time higher energy efficiency compared with conventional catalysis, indicating this strategy is an economical approach to efficient upcycling of plastics towards valuable products. Moreover, the catalyst can tolerate high contaminates, even the landfilled plastics can still be converted to lubricant base oil precursors, which has never been reported before.
The recycling of plastic waste has attracted increasing attention on account of its negative effects on the ecological environment and human health. Photoreforming is emerging as a green and promising approach to upcycle plastic waste into high valuable chemicals as well as H2 fuels. Herein, an earth abundant Ni2P/ZnIn2S4 catalyst prepared by mechanical grinding is reported to selectively photoreform various polyester plastics into high-added-value chemicals coupling with H2 evolution under mild conditions. In particular, polylactic acid (PLA) can be upcycled to pyruvic acid (PA) with high activity (745.9 μmolg-1h-1) and selectivity (> 90%), meanwhile, the H2 evolution rate can reach up to 781.3 μmolg-1h-1 catalyzed by 7.5 wt% Ni2P/ZnIn2S4. This system exhibits excellent photocatalytic performance, benefiting from the efficient photogenerated charge carrier separation and transfer between Ni2P and ZnIn2S4. This work provides a viable and promising solution to simultaneously produce high-purity H2 and added-value chemicals from polyester plastic waste, demonstrating its potential for practical recycling application.
The rational design of visible‐light‐responsive catalysts is crucial for converting solar energy into hydrogen energy to promote sustainable energy development. In this work, a C─S─C bond is introduced into g‐C3N4 (CN) through S doping. With the help of the flexible C─S─C bond under specific stimuli, a hollow coral‐like porous structure of S‐doped g‐C3N4 (S‐CN) is synthesized for the first time. And an S‐doped g‐C3N4/ZnIn2S4 (S‐CN/ZIS) heterojunction catalyst is in situ synthesized based on S‐CN. S0.5‐CN/ZIS exhibits excellent photocatalytic hydrogen evolution (PHE) efficiency (19.25 mmol g−1 h−1), which is 2.7 times higher than that of the g‐C3N4/ZnIn2S4 (CN/ZIS) catalyst (8.46 mmol g−1 h−1), with a high surface quantum efficiency (AQE) of 34.43% at 420 nm. Experiments and theoretical calculations demonstrate that the excellent photocatalytic performance is attributed to the larger specific surface area and porosity, enhanced interfacial electric field (IEF) effect, and appropriate hydrogen adsorption Gibbs free energy (ΔGH*). The synergistic effect of S doping and S‐scheme heterojunction contributes to the above advancement. This study provides new insights and theoretical basis for the design of CN‐based photocatalysts.