| Title | Mining the Carbon Intermediates in Plastic Waste Upcycling for Constructing C-S Bond |
|---|---|
| ID_Doc | 12834 |
| Authors | Kang, HX; He, D; Turchiano, C; Yan, XX; Chai, JT; Weed, M; Elliott, GI; Onofrei, D; Pan, XQ; Xiao, XH; Gu, J |
| Title | Mining the Carbon Intermediates in Plastic Waste Upcycling for Constructing C-S Bond |
| Year | 2024 |
| Published | Journal Of The American Chemical Society, 146.0, 27 |
| Abstract | Postconsumer plastics are generally perceived as valueless with only a small portion of plastic waste being closed-loop recycled into similar products while most of them are discarded in landfills. Depositing plastic waste in landfills not only harms the environment but also signifies a substantial economic loss. Alternatively, constructing value-added chemical feedstocks via mining the waste-derived intermediate species as a carbon (C) source under mild electrochemical conditions is a sustainable strategy to realize the circular economy. This proof-of-concept work provides an attractive "turning trash to treasure" strategy by integrating electrocatalytic polyethylene terephthalate (PET) plastic upcycling with a chemical C-S coupling reaction to synthesize organosulfur compounds, hydroxymethanesulfonate (HMS). HMS can be produced efficiently (Faradaic efficiency, FE of similar to 70%) via deliberately capturing electrophilic intermediates generated in the PET monomer (ethylene glycol, EG) upcycling process, followed by coupling them with nucleophilic sulfur (S) species (i.e., SO32- and HSO3-). Unlike many previous studies conducted under alkaline conditions, PET upcycling was performed over an amorphous MnO2 catalyst under near-neutral conditions, allowing for the stabilization of electrophilic intermediates. The compatibility of this strategy was further investigated by employing biomass-derived compounds as substrates. Moreover, comparable HMS yields can be achieved with real-world PET plastics, showing its enormous potential in practical application. Lastly, Density function theory (DFT) calculation reveals that the C-C cleavage step of EG is the rate-determining step (RDS), and amorphous MnO2 significantly decreases the energy barriers for both RDS and C-S coupling when compared to the crystalline counterpart. |
| https://pubs.acs.org/doi/pdf/10.1021/jacs.4c05512 |
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