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. 2024 Jul 10;16(27):34973-34987.
doi: 10.1021/acsami.4c05315. Epub 2024 Jun 25.

Enhanced Selective Degradation of Pharmaceutical and Personal Care Products by β-Cyclodextrin-Decorated ZIF-67 Nanocomposites in Reclaimed Water

Xi Quan  1 , Yifan Chen  1 , Linlin Yin  1 , Wei Zuo  1 , Yu Tian  1 , Jun Zhang  1   2
Affiliations

Enhanced Selective Degradation of Pharmaceutical and Personal Care Products by β-Cyclodextrin-Decorated ZIF-67 Nanocomposites in Reclaimed Water

Xi Quan et al. ACS Appl Mater Interfaces. .

Abstract

A peroxymonosulfate oxidation system was developed via modification of β-cyclodextrin (β-CD) on the surface of Fe2+-doped ZIF-67 (CD/Fe@ZIF-67) as an activator. The 99.7% carbamazepine, 91.3% bisphenol A (BPA), and 95.4% diclofenac (DCF) degradation efficiency were achieved within 10 min, 60, and 1 min, respectively. The hydrophobicity of these three pollutants is positively correlated with their adsorption kinetic constants by CD/Fe@ZIF-67 due to the introduction of β-CD. Scavenger experiments and electron spin resonance spectra confirmed that carbamazepine was preferentially oxidized by SO4•- [λ(SO4•-)(70.5%) > λ(•OH)(28.2%) > λ(O2•-)(1.3%)], where SO4•- and O2•- played dominant roles in the degradation of BPA [λ(SO4•-)(71.7%) > λ(O2•-)(22.8%) > λ(•OH)(5.5%)], and O2•- was responsible for DCF removal [λ(O2•-) = 93.2%]. Additionally, the particulate catalyst was immobilized in the shell side of a ceramic membrane in a membrane reactor for catalyst recovery. This reactor achieved nearly 100% removal efficiency under optimal conditions: 0.036 wt % catalyst loading, 0.5 mM peroxymonosulfate concentration, 1 L inflow, 10 mg/L initial carbamazepine concentration, and 0.012 L/min hydraulic retention time. In summary, this study elucidates the active role of β-CD in a polymetallic/peroxymonosulfate system and provides valuable insights into the development of effective oxidation methods for pharmaceutical and personal care products in wastewater.

Keywords: Fe@ZIF-67; peroxymonosulfate activation; synergistic catalysis; tube-in-tube membrane reactor; β-cyclodextrin.

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