TY - JOUR
T1 - Encapsulation of Carbon-Nanodots into Metal-Organic Frameworks for Boosting Photocatalytic Upcycling of Polyvinyl Chloride Plastic
AU - Qin, Jibo
AU - Dou, Yibo
AU - Zhou, Jianchi
AU - Zhao, Dan
AU - Orlander, Tobias
AU - Andersen, Henrik Rasmus
AU - Hélix-Nielsen, Claus
AU - Zhang, Wenjing
PY - 2024
Y1 - 2024
N2 - Although polyvinyl chloride (PVC) ranks as the third most mass-produced synthetic plastic, the chemical upcycling of non-biodegradable PVC waste remains a significant challenge. Herein, carbon nanodots combined with the metal-organic framework (CDs/Zr-MOF) are fabricated for photocatalytic upcycling of PVC. Specifically, the ultra-small-sized CDs (~2.0 nm) are encapsulated into Zr-MOF pores via a mild pyrolysis strategy. The maintained MOF structure facilitates charge/mass transfer and improves the surface-to-volume ratio of active sites of CDs. The CDs/Zr-MOF exhibits high activity for PVC conversion of ~76.5% towards acetic acid with a yield of ~14%. The mechanism investigation indicates the generated •OH radicals can efficiently trigger cleavage of C-Cl/C-C bonds of PVC. Moreover, the reduction of the energy barrier for the hydroxylation reaction as a rate-limiting step contributed to improved PVC conversion performance. This work offers a feasible method for fabricating nanoparticle-embedded MOF-based photocatalysts and provides new insights into the chemical upcycling of plastics.
AB - Although polyvinyl chloride (PVC) ranks as the third most mass-produced synthetic plastic, the chemical upcycling of non-biodegradable PVC waste remains a significant challenge. Herein, carbon nanodots combined with the metal-organic framework (CDs/Zr-MOF) are fabricated for photocatalytic upcycling of PVC. Specifically, the ultra-small-sized CDs (~2.0 nm) are encapsulated into Zr-MOF pores via a mild pyrolysis strategy. The maintained MOF structure facilitates charge/mass transfer and improves the surface-to-volume ratio of active sites of CDs. The CDs/Zr-MOF exhibits high activity for PVC conversion of ~76.5% towards acetic acid with a yield of ~14%. The mechanism investigation indicates the generated •OH radicals can efficiently trigger cleavage of C-Cl/C-C bonds of PVC. Moreover, the reduction of the energy barrier for the hydroxylation reaction as a rate-limiting step contributed to improved PVC conversion performance. This work offers a feasible method for fabricating nanoparticle-embedded MOF-based photocatalysts and provides new insights into the chemical upcycling of plastics.
KW - Polyvinyl chloride
KW - Mild pyrolysis
KW - CDs/Zr-MOF photocatalyst
KW - Acetic acid
U2 - 10.1016/j.apcatb.2023.123355
DO - 10.1016/j.apcatb.2023.123355
M3 - Journal article
SN - 0926-3373
VL - 341
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 123355
ER -