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生物合成针铁矿还原氧化石墨烯复合材料协同类 Fenton 催化降解磺胺。

Synergistic catalytic Fenton-like degradation of sulfanilamide by biosynthesized goethite-reduced graphene oxide composite.

机构信息

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.

出版信息

J Hazard Mater. 2021 Aug 5;415:125704. doi: 10.1016/j.jhazmat.2021.125704. Epub 2021 Mar 22.

Abstract

A series of goethite (Gt)-graphene (rGO) composites (Gt-rGO) having different rGO contents (2%-10%) was biologically prepared under mild conditions with Acidovorax sp. BoFeN1 and exhibited comparable or even higher catalytic efficiencies upon sulfonamides degradation than most known chemically synthesized catalysts. Pseudo-first-order rate constant of sulfanilamide degradation (60 μM, 0.971 h) in the system mediated by Gt-rGO with the optimal rGO content of 6% was 6.7, 15.4 and 168.1 folds higher than those in the control rGO/HO, Gt/HO and HO systems, respectively. Excellent synergistic catalytic effects between Gt and rGO in Gt-rGO were identified in four continuous cycles. The Gt-rGO systems exhibited more efficient •OH generation, HO decomposition and Fe(II) accumulation rates than the control Gt or rGO systems. Fast Fe(III)/Fe(II) cycling was obtained in the Gt-rGO systems, which might be due to the strong Fe-C coordination and the decrease of rGO aggregation and Gt particle sizes. Additionally, Gt particles in Gt-rGO exposed more defects as active sites for HO activation. High-performance liquid chromatography-mass spectrometer analysis suggested that sulfanilamide was gradually degraded through hydroxylation, C-N cleavage and benzene ring opening. The results provided a new approach for the tailored design of eco-friendly, cost-effective and efficient iron (oxyhydr)oxides-graphene catalysts for contaminants elimination.

摘要

一系列具有不同还原氧化石墨烯(rGO)含量(2%-10%)的针铁矿(Gt)-还原氧化石墨烯(rGO)复合材料(Gt-rGO)在温和条件下通过 Acidovorax sp. BoFeN1 生物制备,并在磺胺类降解方面表现出可比甚至更高的催化效率,优于大多数已知的化学合成催化剂。在由最佳 rGO 含量为 6%的 Gt-rGO 介导的系统中,磺胺降解的拟一级速率常数(60 μM,0.971 h)为 6.7、15.4 和 168.1 倍,分别高于对照 rGO/HO、Gt/HO 和 HO 系统中的速率常数。在四个连续循环中,Gt-rGO 中 Gt 和 rGO 之间存在优异的协同催化作用。Gt-rGO 系统比对照 Gt 或 rGO 系统具有更高的 •OH 生成、HO 分解和 Fe(II)积累速率。在 Gt-rGO 系统中获得了快速的 Fe(III)/Fe(II)循环,这可能是由于强的 Fe-C 配位以及 rGO 聚集和 Gt 颗粒尺寸的减小。此外,Gt-rGO 中的 Gt 颗粒暴露了更多的缺陷作为 HO 活化的活性位点。高效液相色谱-质谱分析表明,磺胺逐渐通过羟化、C-N 断裂和苯环开环降解。这些结果为设计环保、经济高效的铁(氧)氢氧化物-石墨烯催化剂用于去除污染物提供了一种新方法。

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