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Synthesis and assessment of schwertmannite/few-layer graphene composite for the degradation of sulfamethazine in heterogeneous Fenton-like reaction.

ABSTRACT: Schwertmannite (sch), an iron oxyhydrosulfate mineral, can catalyse a Fenton-like reaction to degrade organic contaminants, but the reduction of Fe(III) to Fe(II) on the surface of schwertmannite is a limiting step for the Fenton-like process. In the present study, the sch/few-layer graphene (sch-FLG) composite was synthesized to promote the catalytic activity of sch in a Fenton-like reaction. It was found that sch can be successfully carried by FLG in sch-FLG composite, mainly via the chemical bond of Fe-O-C on the surface of sch-FLG. The sch-FLG exhibited a much higher catalytic activity than sch or FLG for the degradation of sulfamethazine (SMT) in the heterogeneous Fenton-like reaction, which resulted from the fact that the FLG can pass electrons efficiently. The degradation efficiency of SMT was around 100% under the reaction conditions of H2O2 200-500 mg l-1, sch-FLG dosage 1-2 g l-1, temperature 28-38°C, and initial solution pH 1-9. During the repeated uses of sch-FLG in the Fenton-like reaction, it maintained a certain catalytic activity for the degradation of SMT and the mineral structure was not changed. In addition, SMT may be finally mineralized in the Fenton-like reaction catalysed by sch-FLG, and the possible degradation pathways were proposed. Therefore, the sch-FLG is an excellent catalyst for SMT degradation in a heterogeneous Fenton-like reaction.

SUBMITTER: Wang D

PROVIDER: S-EPMC7428258 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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Synthesis and assessment of schwertmannite/few-layer graphene composite for the degradation of sulfamethazine in heterogeneous Fenton-like reaction.

Wang Dianzhan D Gu Ye Y Yang Zhaoshun Z Zhou Lixiang L

Royal Society open science 20200722 7

Schwertmannite (sch), an iron oxyhydrosulfate mineral, can catalyse a Fenton-like reaction to degrade organic contaminants, but the reduction of Fe(III) to Fe(II) on the surface of schwertmannite is a limiting step for the Fenton-like process. In the present study, the sch/few-layer graphene (sch-FLG) composite was synthesized to promote the catalytic activity of sch in a Fenton-like reaction. It was found that sch can be successfully carried by FLG in sch-FLG composite, mainly via the chemical ...[more]

PMID: 32874605

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Project description:The mechanism for the functionalization of graphene layers with pyrrole compounds was investigated. Liquid 1,2,5-trimethylpyrrole (TMP) was heated in air in the presence of a high surface area nanosized graphite (HSAG), at temperatures between 80 °C and 180 °C. After the thermal treatments solid and liquid samples, separated by centrifugation, were analysed by means of Raman, Fourier Transform Infrared (FT-IR) spectroscopy, X-Rays Photoelectron Spectroscopy (XPS) and ¹H-Nuclear Magnetic Resonance (¹H NMR) spectroscopy and High Resolution Transmission Electron Microscopy (HRTEM). FT-IR spectra were interpreted with the support of Density Functional Theory (DFT) quantum chemical modelling. Raman findings suggested that the bulk structure of HSAG remained substantially unaltered, without intercalation products. FT-IR and XPS spectra showed the presence of oxidized TMP derivatives on the solid adducts, in a much larger amount than in the liquid. For thermal treatments at T ≥ 150 °C, IR spectral features revealed not only the presence of oxidized products but also the reaction of intra-annular double bond of TMP with HSAG. XPS spectroscopy showed the increase of the ratio between C(sp²)N bonds involved in the aromatic system and C(sp³)N bonds, resulting from reaction of the pyrrole moiety, observed while increasing the temperature from 130 °C to 180 °C. All these findings, supported by modeling, led to hypothesize a cascade reaction involving a carbocatalyzed oxidation of the pyrrole compound followed by Diels-Alder cycloaddition. Graphene layers play a twofold role: at the early stages of the reaction, they behave as a catalyst for the oxidation of TMP and then they become the substrate for the cycloaddition reaction. Such sustainable functionalization, which does not produce by-products, allows us to use the pyrrole compounds for decorating sp² carbon allotropes without altering their bulk structure and smooths the path for their wider application.

Dataset Information

Synthesis and assessment of schwertmannite/few-layer graphene composite for the degradation of sulfamethazine in heterogeneous Fenton-like reaction.

Publications

Synthesis and assessment of schwertmannite/few-layer graphene composite for the degradation of sulfamethazine in heterogeneous Fenton-like reaction.

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