Enhancement of Fe@porous carbon to be an efficient mediator for peroxymonosulfate activation for oxidation of organic contaminants: Incorporation NH2-group into structure of its MOF precursor

Chao Liu, Yiping Wang, Yuting Zhang, Ruoyu Li, Weidong Meng, Zilong Song, Fei Qi, Bingbing Xu, Wei Chu, Donghai Yuan, Bin Yu

Research output: Journal article publicationJournal articleAcademic researchpeer-review

40 Citations (Scopus)

Abstract

Metal-organic frameworks (MOFs) derived metal@porous carbon showed good performance in peroxymonosulfate (PMS) activation for refractory organic chemical degradation from aqueous. However, the effect of structure and physical-chemical properties of metal@porous carbon on PMS activation and its involved reaction mechanism were still unclear. Herein, Fe@porous carbon derived from MOF MIL-53(Fe) was used as target, to discuss the role of NH2-group incorporation on the development of structure and physical-chemical properties of obtained Fe@porous carbon, and reaction mechanism for PMS activation. The incorporation of NH2-group significantly decreased the synthesis temperature of Fe@porous carbon and increased the encapsulation of Fe0 in the porous carbon. Furthermore, the addition of nitrogen in porous carbon and rigid encapsulation structure reduced the defects of the Fe@porous carbon. These improvements of the structure and chemical properties were favored for enhancement of the catalytic activity and stability of the obtained Fe@porous carbon in the activation of PMS. Electron paramagnetic resonance (EPR) experiments indicated that SO4 [rad]−, [rad]OH and 1O2 were involved. The radical pathway involving SO4 [rad]− and [rad]OH was the prevailing pathway while the nonradical pathway involving 1O2 was the recessive pathway. Based on intermediate identification, the degradation pathway of acyclovir (ACV) was proposed as SO4 [rad]− and [rad]OH derived process, and eight of intermediates were first reported. It was interesting to note that iron species, carbon structure, and nitrogen element in the catalysts derived from MIL-53(Fe) or NH2-MIL-53(Fe) clearly showed different role and reaction pathway. This work not only provided an efficient Fe@N-doped porous carbon for activation PMS to degrade refractory organic chemicals for water purification, but also suggested a valuable insight for the design of metal@porous carbon derived from MOF.

Original languageEnglish
Pages (from-to)835-848
Number of pages14
JournalChemical Engineering Journal
Volume354
DOIs
Publication statusPublished - 15 Dec 2018

Keywords

  • Acyclovir
  • Fe@porous carbon
  • Metal-organic frameworks
  • Peroxymonosulfate
  • Sulfate radical

ASJC Scopus subject areas

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

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