4.7 Article

A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine

Journal

ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
Volume 28, Issue 39, Pages 55014-55028

Publisher

SPRINGER HEIDELBERG
DOI: 10.1007/s11356-021-14714-8

Keywords

Enhanced kinetic; Surface reaction; Pharmaceutical; Graphene oxide; Magnetite; Radical reaction

Funding

  1. Sao Paulo Research Foundation [2014/50945-4, 2018/17517-0]
  2. National Council for Scientific and Technological Development (CNPq) [465571/2014-0]
  3. Coordination for the Improvement of Higher Education Personnel (CAPES) [88887136426/2017/00]
  4. Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP) [18/17517-0, 14/50945-4] Funding Source: FAPESP

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The study found that graphene oxide-magnetite nanocomposites as catalysts in the heterogeneous Fenton process showed significantly improved catalytic activity in the degradation of caffeine, with a synergistic effect of up to 17.1 times and complete removal achieved within 90 minutes. Improved mass transfer, adsorption, efficient degradation, and enhanced HO center dot generation were attributed to the interaction between the phases, highlighting the important role of graphene oxide in the degradation kinetics of the process.
Two compositions of graphene oxide-magnetite nanocomposites were studied as catalysts in the heterogeneous Fenton process. Transmission electron microscopy and X-ray diffraction revealed that the graphene oxide sheets were covered with nanoparticles of magnetite, with an average crystallite size of 7 nm. Infrared spectroscopy analysis indicated that the phases interacted through covalent Fe-O-C bonds. The composites presented significantly improved catalytic activity, compared to pure magnetite, with a synergistic effect of up to a factor of 17.1 for the Fenton degradation of caffeine, achieving total removal after 90 min. This synergistic effect was a consequence of the interaction between the phases, resulting in improved mass transfer of caffeine to the catalyst surface, adsorption and efficient degradation, with enhanced HO center dot generation. The surface reaction constant increased by up to three orders of magnitude, demonstrating the important role of graphene oxide in the degradation kinetics of the heterogeneous Fenton process. The surface-bonded hydroxyl radicals were responsible for caffeine degradation, achieving 9.4 mu mol L-1. After five degradation cycles, a loss of Fe-O-C bonds and increase in oxygenated groups were associated with a small decrease of caffeine removal efficiency, from 98 to 82%, without significant iron leaching, in the dark, and with low consumption of hydrogen peroxide.

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