Bio-Inspired Cascade Photocatalysis on Fe Single-Atom Carbon Nitride Upcycles Plastic Wastes for Effective Acetic Acid Production

Journal Article · Fri Dec 26 00:00:00 UTC 2025 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202505453 · OSTI ID:3374579

Wei, Wei; Du, Cheng; Ge, Jiawei; Wang, Xiang; Chen, Zuolong; Zhang, Meng; Guo, Tao; Wang, Lei; Wang, Maoyu; Liu, Yuzi; Zhou, Hua; Sun, Chengjun; Chen, Ning; Chen, Weifeng; Billinghurst, Brant; Shakourian-Fard, Mehdi; Sprenger, Peter; Fani Sani, Fatemeh; Quan, Yulian; Kendall, Brian ; Brouwer, Roy; Wu, Yimin A.

Plastic imposes a critical threat to the environment, ecosystems and human health, because of low utilization efficiency of plastics. Here, we demonstrate a sustainable highly efficient cascade photocatalysis for upcycle plastics to value-added acetic acid using Fe single atom catalysts (Fe@C3N4 SAC) at ambient conditions. Inspired by Phanerochaete chrysosporium microbial, the defected Fe@C3N4 SAC acts as a as a bifunctional cascade photocatalyst for both Fenton-like and CO2 reduction reactions. During the reaction, hydroxyl radicals (*OH) form and subsequently oxidize plastics into CO2 intermediates. These CO2 intermediates were then photo-reduced to CH3COOH on the same catalyst via cascade photocatalysis. The mechanism was confirmed by in situ multimodal microscopy and spectroscopies, with density functional theory calculations. A state-of-art CH3COOH yield of 63.8 mg h-1 gcat-1 from PVC, 12.7 mg h-1 gcat-1 from PE, 5.4 mg h-1 gcat-1 from PET, and 5.3 mg h-1 gcat-1 from PP were directly obtained under AM1.5G solar irradiation and further validated under real sunlight (~ 0.6 sun), achieving 5.6 mg h-1 gcat-1 from PET, using low-cost Fe@C3N4 SAC in a sealed reactor by enhancing the photon transport and utilization efficiency. The techno-economic analysis shows it is promising to practically mitigate plastic based on broader social welfare assessments.

• Research Organization: Argonne National Laboratory (ANL)
• Sponsoring Organization: Natural Sciences and Engineering Research Council of Canada (NSERC); US Department of Energy; USDOE Office of Science - Office of Basic Energy Sciences - Scientific User Facilities Division
• Grant/Contract Number: AC02-06CH11357
• OSTI ID: 3374579
• Journal Information: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 9 Vol. 16; ISSN 1614-6832
• Country of Publication: United States
• Language: English