Single-Atom Photocatalyst as Floatable Artificial Leaf for Upcycling Oceanic Plastic Waste.

Talebian-Kiakalaieh, Amin; Xu, Xin; Ji, Wenzhong; Liu, Yun; Xia, Bingquan; Ran, Jingrun; Qiao, Shi-Zhang · Adv Mater · 2026

basic_science · Level V

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Abstract

Over ∼8 billion tons of plastic have been produced to date, with ∼80% of them ended up in landfills/oceans. Among them, polypropylene (PP) possesses the lowest global recycling rate (< 1%). To resolve this, Ru single atoms (SAs) loaded photocatalysts (ZnIn<sub>2</sub>S<sub>4</sub>/Ru SAs) in the forms of powder/floatable artificial leaf (AL) were prepared for direct conversion of raw PP plastic into valuable chemicals. The optimized photocatalyst exhibits exceptional performance with a total formic/acetic acid production of 1022.5 µmol g<sup>-1</sup>. In situ X-ray photoelectron spectroscopy, in situ atomic force microscopy-kelvin probe force microscopy, and in situ electron paramagnetic resonance (EPR) reveal efficient electron extraction from ZnIn<sub>2</sub>S<sub>4</sub> nanosheets to Ru SAs, with subsequent electron capture by O<sub>2</sub> molecules in air. Additionally, in situ transient-state photoluminescence spectroscopy, transient photovoltage measurement, and in situ EPR unveil the electrolyte-assisted polarization (induced by cations/anions in seawater) significantly enhancing charge separation/transfer. Finally, in situ EPR, in situ infrared (IR) spectroscopy, and quenching experiments corroborate the pivotal roles of reactive oxygen species (·O<sub>2</sub> <sup>-</sup>/·OH) for upcycling PP into valuable chemicals. These results highlight the transformative potential of floatable AL concept for converting plastic waste into high-value chemicals, offering a sustainable solution to plastic contamination.