4.7 Article

Activation of peroxydisulfate by biogenic nanocomposites of reduced graphene oxide and goethite for non-radical selective oxidation of organic contaminants: Production of singlet oxygen and direct electron transfer

期刊

CHEMICAL ENGINEERING JOURNAL
卷 430, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133177

关键词

Peroxydisulfate; Non-radical oxidation; Singlet oxygen; Direct electron transfer; Selective reactivity

资金

  1. National Natural Science Foundation of China [21876023]
  2. Programme of Introducing Talents of Discipline to Universities [B13012]

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In this study, biologically prepared Gt-rGO nanocomposites exhibit efficient catalytic activity in activating PDS for organic pollutants degradation, showing higher rate constants compared to other systems. The nanocomposites show high stability and generate singlet oxygen, effectively accelerating electron transfer in the PDS system. This indicates their potential for efficient removal of organic pollutants.
Composites of carbon nanomaterials and nanosized iron oxides have been extensively investigated as efficient catalysts for H2O2 decomposition in advanced oxidation. However, little is known about their catalytic activity and mechanism in peroxydisulfate (PDS) activation. In this study, reduced graphene oxide (rGO) and goethite (Gt) nanocomposites (Gt-rGO) with different rGO contents were biologically prepared and their abilities of activating PDS for elimination of organic pollutants were investigated. In 4 h, 97.5% of sulfanilamide (SA, 20 mu M) was efficiently degraded in the Gt-rGO/PDS system. The pseudo-first-order rate constant of SA degradation in the Gt-rGO/PDS system (0.682 h-1) was 6.3, 22.7, and 25.3 folds higher than those in the control rGO/PDS, Gt/PDS, and PDS systems, respectively. The nanocomposites maintained high stability and exhibited excellent catalytic effects on SA degradation over four continuous cycles. Quenching experiments and electron spin resonance results verified that singlet oxygen was generated in the Gt-rGO/PDS system. Additionally, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and electrochemical experiments demonstrated that Gt-rGO acting as mediator directly accelerated electron transfer between organic pollutants and PDS. Based on the non-radical oxidation mechanism, a selective reactivity of the Gt-rGO/PDS system toward organic pollutants possessing different ionization potentials was shown. Biogenic C-Fe nanocomposites prepared under growing conditions present new potentials for efficient activation of persulfates and effective removal of SA and other organic pollutants.

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