Novel carbon based Fe-Co oxides derived from Prussian blue analogues activating peroxymonosulfate: Refractory drugs degradation without metal leaching

Chao Liu, S. Liu, Liyuan Liu, Xing Tian, Longyan Liu, Y. Xia, Xiaoliang Liang, Yiping Wang, Zilong Song, Yuting Zhang, R. Li, Ye Liu, Fei Qi, Wei Chu, Daniel C.W. Tsang, Bingbing Xu, Hui Wang, Amir lkhlaq

Research output: Journal article publicationJournal articleAcademic researchpeer-review

57 Citations (Scopus)

Abstract

To meet the current challenges of removing refractory drugs from wastewater and groundwater, an efficient and environmentally friendly treatment process is desired. Herein, a novel magnetic composite of carbon-based Fe-Co oxide (MCFC) was fabricated from a Prussian blue analogue and graphene oxide by pyrolysis in nitrogen and then re-sintering in air. MCFC showed good performance for several kinds of refractory drugs (including 4-aminobenzoic acid ethyl ester (ABEE), sulfamethoxazole and acyclovir) degradation by activation peroxymonosulfate (PMS), without any detectable metal leaching, as an important green environmental remediation technology. A slight performance decrease of MCFC observed during the reuse, was able to be recovered by a simple thermal process. No metal ions dissolution and thermal regeneration was an important development on PMS activation catalyst. Degradation intermediates of a refractory drug, ABEE, were identified by liquid chromatography quadrupole time-of-flight mass spectrometry. The degradation pathways of ABEE were established, with intermediates being generated by the electrophilic/radical addition and the hydrogen abstraction. At last, PMS activation pathways was proposed as that PMS was activated by Co2+ and Fe2+ on the surface of MCFC, pyrrolic-N, pyridinic-N, and carbonyl groups, to form singlet oxygen (1O2), hydroxyl radicals ([rad]OH) and sulfate radicals (SO4[rad]−). The synergistic effects between the metal nanocrystals and nitrogen-doped carbon promoted the regeneration of the surface Fe2+ and Co2+, which resulted in F4C6G5-6N-4a showing excellent catalytic activity for PMS activation. Through the above combination of non-radical (1O2) and radical (SO4[rad]− and [rad]OH) processes, ABEE was degraded and mineralized. This work presents a promising green heterogeneous catalyst for the degradation of refractory drugs in municipal wastewater/groundwater by PMS activation.

Original languageEnglish
Article number122274
JournalChemical Engineering Journal
Volume379
DOIs
Publication statusPublished - 1 Jan 2020

Keywords

  • Carbon-based catalyst
  • Metal ions leaching
  • Peroxymonosulfate
  • Prussian blue analogue

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

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