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为了提高磁性纳米粒子在三维还原氧化石墨烯中的非均相芬顿有机染料降解的催化活性。

Toward enhanced catalytic activity of magnetic nanoparticles integrated into 3D reduced graphene oxide for heterogeneous Fenton organic dye degradation.

机构信息

POLYMAT, Facultad de Ciencias, Químicas, University of the Basque Country UPV/EHU, Joxe Mari Korta, Center - Avda. Tolosa, 72, 20018, San Sebastian, Spain.

Organic and Polymer Research Laboratory, Department of Chemistry, Faculty of Science, University of Sistan and Baluchestan, Zahedan, Iran.

出版信息

Sci Rep. 2021 Sep 15;11(1):18343. doi: 10.1038/s41598-021-97712-7.

Abstract

Composite Fenton nanocatalyst was prepared by water-based in situ creation of FeO nanoparticles integrated within the self-assembly 3D reduced graphene oxide (rGO) aerogel. The hybrid applied for the degradation of Acid Green 25 (AG-25) organic dye in an aqueous solution, in the presence of HO. By investigating the conditions that maximize the dye adsorption by the 3D composite, it was found that the pH of the solution should be adjusted between the pKa of the functional groups present on the rGO surface (carboxylic acid) and that of the dye (sulfonic acid) to promote electrostatic interactions dye-3D structure. Performed under these conditions, Fenton degradation of AG-25 in presence of HO was completed in less than 30 min, including all the intermediate products, as demonstrated by MALDI-TOF-MS analysis of the aqueous solution after discoloration. Moreover, this was achieved in a solution with as high a dye concentration of 0.5 mg/mL, with only 10 mg of 3D composite catalyst, at room temperature and without additional energy input. The high performance was attributed to the creation of charge-transfer complex between rGO and FeO nanoparticles throughout covalent bond C-O-Fe, the formation of which was promoted by the in situ synthesis procedure. For the first time, up to the authors' knowledge, AG-25 degradation mechanism was proposed.

摘要

复合芬顿纳米催化剂是通过在自组装的 3D 还原氧化石墨烯 (rGO) 气凝胶内原位生成 FeO 纳米颗粒制备的。该杂化材料应用于在水溶液中 HO 的存在下降解酸性绿 25 (AG-25) 有机染料。通过研究最大程度提高 3D 复合材料对染料吸附的条件,发现溶液的 pH 值应调节到 rGO 表面存在的官能团(羧酸)的 pKa 和染料(磺酸)的 pKa 之间,以促进静电相互作用染料-3D 结构。在这些条件下,在 HO 存在下进行 Fenton 降解 AG-25 在不到 30 分钟内完成,包括所有中间产物,如通过 MALDI-TOF-MS 分析褪色后水溶液得到证实。此外,这是在 0.5 mg/mL 高浓度染料溶液中,在室温下,仅使用 10 mg 3D 复合催化剂,无需额外的能量输入即可实现。高性能归因于 rGO 和 FeO 纳米颗粒之间形成的电荷转移复合物,通过原位合成过程促进了这种复合物的形成。据作者所知,这是首次提出 AG-25 降解机制。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c0a9/8443561/774e307090dc/41598_2021_97712_Fig1_HTML.jpg

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