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通过简便的热处理含铁蜡烛烟灰合成 Fe/FeO@多孔碳,用于过一硫酸盐活化和高效降解磺胺甲恶唑。

Synthesis of Fe/FeO@porous carbon through a facile heat treatment of iron-containing candle soots for peroxymonosulfate activation and efficient degradation of sulfamethoxazole.

机构信息

School of Environmental and Civil Engineering, Jiangnan University, Wuxi, Jiangsu, China; Jiangsu Key Laboratory of Anaerobic Biotechnology, Wuxi, Jiangsu, China.

School of Environmental and Civil Engineering, Jiangnan University, Wuxi, Jiangsu, China; Jiangsu Key Laboratory of Anaerobic Biotechnology, Wuxi, Jiangsu, China; Jiangsu Engineering Laboratory for Biomass Energy and Carbon Reduction Technology, China.

出版信息

J Hazard Mater. 2021 Jun 5;411:124952. doi: 10.1016/j.jhazmat.2020.124952. Epub 2020 Dec 24.

Abstract

Developing highly efficient, reusable, non-toxic and low-cost catalysts is of great importance for persulfate-based advanced oxidation processes (AOPs). In this work, ferrocene was mixed into paraffin to prepare a candle, and the iron-containing candle soots were collected and heated at 500 °C~900 °C under N atmosphere for 1 h to prepare magnetically recyclable Fe/FeO@porous carbon (Fe/FeO@PC) catalysts. The Fe/FeO@PC-700 obtained after pyrolysis at 700 °C exhibited the best catalytic activity for sulfamethoxazole (SMX) degradation. 10 mg/L SMX could be completely degraded within 10 min by 0.2 g/L of Fe/FeO@PC-700 and 0.5 mM PMS at pH 5.0. The carbon shell effectively inhibited the Fe leaching of Fe/FeO@PC-700, and 99.73% of Fe was retained after five consecutive cycles. In the Fe/FeO@PC-700/PMS system, SMX was degraded through the sulfate radical (SO·), hydroxyl radical (·OH), superoxide radical (O·) dominated radical pathway, and the singlet oxygen (O) dominated non-radical pathway. The coexisting inorganic ions and natural organic matters (NOM) in actual water inhibited the degradation of SMX. Finally, four possible degradation pathways were proposed based on the degradation intermediates of SMX. This work provides a facile heat treatment of iron-containing candle soots strategy to prepare the metal@carbon catalysts for PMS-based AOP.

摘要

开发高效、可重复使用、无毒且低成本的催化剂对于基于过硫酸盐的高级氧化工艺(AOPs)至关重要。在这项工作中,将二茂铁混入石蜡中制备蜡烛,收集含铁的蜡烛烟灰,并在 N 气氛下于 500°C~900°C 下加热 1 小时,以制备可磁回收的 Fe/FeO@多孔碳(Fe/FeO@PC)催化剂。在 700°C 下热解得到的 Fe/FeO@PC-700 对磺胺甲恶唑(SMX)的降解表现出最佳的催化活性。在 pH 5.0 下,0.2g/L 的 Fe/FeO@PC-700 和 0.5mM 的过一硫酸盐(PMS)可在 10 分钟内完全降解 10mg/L 的 SMX。碳壳有效地抑制了 Fe/FeO@PC-700 的铁浸出,五次连续循环后保留了 99.73%的铁。在 Fe/FeO@PC-700/PMS 体系中,SMX 通过硫酸根自由基(SO·)、羟基自由基(·OH)、超氧自由基(O·)主导的自由基途径和单线态氧(O)主导的非自由基途径降解。实际水中共存的无机离子和天然有机物(NOM)抑制了 SMX 的降解。最后,根据 SMX 的降解中间产物提出了四条可能的降解途径。这项工作提供了一种简便的含铁蜡烛烟灰热处理策略,用于制备基于过一硫酸盐的 AOP 的金属@碳催化剂。

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