open access publication

Article, 2024

Encapsulation of carbon-nanodots into metal-organic frameworks for boosting photocatalytic upcycling of polyvinyl chloride plastic

Applied Catalysis B Environmental, ISSN 1873-3883, 0926-3373, Volume 341, Page 123355, 10.1016/j.apcatb.2023.123355

Contributors

Qin, Jibo [1] Dou, Yi-Bo 0000-0003-0802-9898 (Corresponding author) [2] Zhou, Jianchi [2] Zhao, Dan 0000-0003-3822-1418 [1] Orlander, Tobias 0000-0001-8701-5376 [1] Andersen, Henrik Rasmus 0000-0002-7013-9193 [1] Hélix-Nielsen, Claus 0000-0002-9392-7133 [1] Zhang, Wenjing 0000-0002-5011-1951 (Corresponding author) [1]

Affiliations

  1. [1] Technical University of Denmark
  2. [NORA names: DTU Technical University of Denmark; University; Denmark; Europe, EU; Nordic; OECD];
  3. [2] Beijing University of Chemical Technology
  4. [NORA names: China; Asia, East]

Abstract

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.

Keywords

Cd, MOF structure, MOF-based photocatalysts, PVC waste, Zr-MOFs, acetic acid, acid, activity, barriers, carbon, carbon nanodots, charge/mass, charge/mass transfer, chemical, chemical upcycling, chloride, conversion, conversion performance, encapsulation, energy, energy barrier, framework, hydroxyl, hydroxylation reaction, investigation, mechanism, mechanism investigation, metal-organic frameworks, method, nanodots, performance, photocatalyst, plasticity, polyvinyl, polyvinyl chloride, polyvinyl chloride plastics, pore, pyrolysis strategy, radicals, reaction, reduction, sites of CD, strategies, structure, surface-to-volume ratio, synthetic plastics, transfer, triggers cleavage, upcycling, waste, yield

Funders

  • National Natural Science Foundation of China
  • China Scholarship Council
  • Innovation Fund Denmark
  • Novo Nordisk Foundation

Data Provider: Digital Science