4.7 Article

Kinetics and mechanisms of enhanced degradation of ibuprofen by piezo-catalytic activation of persulfate

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 392, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.123818

Keywords

Piezo-catalysis; Sulfate radicals; Persulfate activation; Ibuprofen; Degradation pathway

Funding

  1. National Natural Science Foundation of China [51578556, 21876212, 41603097, 41573086]
  2. Natural Science Foundation of Guangdong Province [2015A030308005, S2013010012927, S2011010003416]
  3. Science and Technology Research Programs of Guangdong Province [2014A020216009]
  4. Fundamental Research Funds for the Central Universities [19lgpy157, 13lgjc10]
  5. Start-up Funds for High-Level Talents of Sun Yat-sen University [38000-18841203]
  6. Guangzhou Science and Technology Program [201904010353]
  7. Guangdong Basic and Applied Basic Research Foundation [2019A1515011015]
  8. Shanghai Tongji Gao Tingyao Environmental Science and Technology Development Foundation (STGEF)

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This study investigates the degradation of a refractory emerging contaminant (i.e., ibuprofen) by a newly developed piezoelectric catalytic persulfate (PS) activation process. BaTiO3 nanoparticles (NP) and nanowires (NW) were hydrothermally synthesized and used as the piezo-catalysts to activate PS under ultrasonic irradiation for radical generation and ibuprofen (IBP) degradation. IBP was efficiently degraded in the US/BTO NW/PS system with a pseudo first order rate constant of 0.0818 min(-1), and the rate constant was faster than that in the US/BTO NP/PS (0.0492 min(-1)), US/BTO NW (0.0324 min(-1)) and US/PS (0.0057 min(-1)) systems. The outstanding performance of IBP degradation in the US/BTO NW/PS system was attributed to the continuous generation of center dot SO4- and center dot OH via PS activation by the piezo-catalysis induced electrons. center dot SO4- and center dot OH contributed 53% and 44% to the IBP degradation respectively. Meanwhile, center dot O-2, O-1(2) and H2O2 were in-situ formed and identified as key intermediates for the generation of SO4- and center dot OH. The IBP was partially mineralized and transformed to other organic compounds. The degradation products were identified using the UPLC/ESI-tqMS and a degradation pathway was proposed, which involved a sequence of hydroxylation, decarboxylation/demethylation and ring-opening reactions with center dot SO4- and center dot OH. This study demonstrates a new energy-saving approach to activating PS for micropollutant abatement and also provides insights into the mechanisms of the PS activation by the piezoelectric catalysis.

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