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

ACS Appl Mater Interfaces

State Key Laboratory of Urban Water Resource and Environment (SKLUWRE), Joint Research Center of Biomass Energy Development and Utilization, Harbin Institute of Technology, Harbin 150090, China.

Published: July 2024

AI Article Synopsis

  • Researchers developed a peroxymonosulfate oxidation system using modified β-cyclodextrin on Fe-doped ZIF-67, achieving high degradation rates of pollutants like carbamazepine (99.7%) and bisphenol A (91.3%) within short time frames.
  • The study found that the effectiveness of pollutant removal was influenced by their hydrophobicity and that different reactive species such as SO and O played varying roles in degrading these compounds.
  • A ceramic membrane reactor was used to immobilize the catalyst, resulting in nearly 100% pollutant removal efficiency under optimized conditions, showcasing the potential for improved treatments of pharmaceutical wastewater.

Article Abstract

A peroxymonosulfate oxidation system was developed via modification of β-cyclodextrin (β-CD) on the surface of Fe-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 SO [λ(SO)(70.5%) > λ(OH)(28.2%) > λ(O)(1.3%)], where SO and O played dominant roles in the degradation of BPA [λ(SO)(71.7%) > λ(O)(22.8%) > λ(OH)(5.5%)], and O was responsible for DCF removal [λ(O) = 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.

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http://dx.doi.org/10.1021/acsami.4c05315DOI Listing

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