Efficient enhancement of ozonation performance via ZVZ immobilized g-C3N4 towards superior oxidation of micropollutants

Chemosphere. 2018 Aug:205:369-379. doi: 10.1016/j.chemosphere.2018.04.121. Epub 2018 Apr 21.

Abstract

A functional organic-metal composite material zero-valent zinc immobilized graphitic carbon nitride (ZVZ-g-C3N4) was prepared by a fast and facile two-step synthetic approach with an optimal ZVZ content of 5.4 wt%. The structure, surface morphology and chemical composition of the as-synthesized ZVZ-g-C3N4 were characterized by BET surface area, XRD, FT-IR, SEM, TEM, and XPS, respectively. ZVZ-g-C3N4 composite exhibited superior catalytic ozonation activity with an improvement of 61.2% on atrazine (ATZ) degradation efficiency in 1.5 min reaction, more than 12 times of the pseudo-first-order rate constant, and almost 16-fold of the Rct value obtained in O3/ZVZ-g-C3N4 process compared to O3 alone. Meanwhile, the ATZ degradation efficiency was gradually enhanced with increasing ZVZ-g-C3N4 dosage and initial solution pH in the range from 3.0 to 9.0, and a higher amount of ATZ was degraded when the initial concentration of ATZ rose from 1 to 10 mg L-1. The enhanced catalytic ozonation activity of ZVZ-g-C3N4 is attributed to the synergistic effects among ZVZ, ZnO and g-C3N4, as well as the improved dispersibility, increased surface area, and intensive electron-transfer ascribed to the electronic and surface properties modification. The radical scavengers experiments demonstrated that O2-, OH, and 1O2 were the dominant reactive radical species in the multifunctional processes. Moreover, an empirical kinetic model was proposed to predict ATZ degradation. The results indicated that the ZVZ-g-C3N4 composite was a highly efficient, recoverable, and durable catalyst, which would provide a promising alternative in catalytic ozonation.

Keywords: Catalytic ozonation; Kinetic study; Reaction mechanism; ZVZ-G-C(3)N(4).

MeSH terms

  • Catalysis
  • Environmental Pollutants / analysis
  • Graphite / chemistry
  • Kinetics
  • Nitriles / chemistry*
  • Oxidation-Reduction
  • Ozone / chemistry*
  • Spectroscopy, Fourier Transform Infrared
  • Surface Properties
  • Zinc / chemistry*

Substances

  • Environmental Pollutants
  • Nitriles
  • cyanogen
  • Ozone
  • Graphite
  • Zinc