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污泥衍生生物炭活化过硫酸盐对2,4-二氯苯酚的高效降解:性能与机制

Persulfate activation by sludge-derived biochar for efficient degradation of 2,4-dichlorophenol: performance and mechanism.

作者信息

Liu Shurui, Wang Jin, Zhang Zijie, Dou Mengmeng, Huo Kaili, Ding Guoyu, Zhou Yanmei, Qiao Chen

机构信息

School of Environment, Beijing Key Laboratory of Aqueous Typical Pollutants Control and Water Quality Safeguard, Beijing Jiaotong University, Haidian District, Beijing, 100044, China.

North China Municipal Engineering Design & Research Institute Co. Ltd., Tianjin, 300074, China.

出版信息

Environ Sci Pollut Res Int. 2023 Mar;30(15):45259-45273. doi: 10.1007/s11356-023-25504-9. Epub 2023 Jan 27.

Abstract

Porous sludge biochar (PSDBC) and zero-valent iron (ZVI) supported on porous sludge biochar composite (ZVI@PSDBC) were synthesized using municipal sludge through pyrolysis under N atmosphere, which manifested upgraded performance in persulfate (PS) activation for 2,4-dichlorophenol (2,4-DCP) degradation. The 2,4-DCP (50 mg/L) could be almost completely removed within 20 min under relatively low PS dosage (0.5 mmol/L) in both PSDBC/PS and ZVI@PSDBC/PS systems, and the mineralization rate could respectively approach 73.7% and 91.6% in 60 min. Combined with a scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) characterization and electron spin-resonance (ESR) detection, electrochemical analysis, the radical and non-radical pathways in the catalytic systems were discussed. Graphitized structure and superior conductivity made PSDBC and ZVI@PSDBC not only act as electron donors in PS activation to create radicals (mainly SO and ·OH), but also as "mediators" to facilitate the direct electron transfer from 2,4-DCP to the catalysts-PS complexes. The C=O groups of PSDBC and ZVI@PSDBC aided in the production of O. Meanwhile, zero-valent iron nanoparticles promoted the formation of radicals as the reactive sites of PS, resulting in the most effective 2,4-DCP degradation in the ZVI@PSDBC/PS system. The stability and practicability of sludge biochar materials had been demonstrated in reusability and actual wastewater experiments. The findings provided a promising way for the reuse of municipal sludge and effective PS activation in wastewater treatment.

摘要

采用城市污泥在氮气气氛下热解合成了多孔污泥生物炭(PSDBC)和负载在多孔污泥生物炭上的零价铁(ZVI)复合材料(ZVI@PSDBC),其在过硫酸盐(PS)活化降解2,4-二氯苯酚(2,4-DCP)方面表现出了提升的性能。在PSDBC/PS和ZVI@PSDBC/PS体系中,相对较低的PS投加量(0.5 mmol/L)下,2,4-DCP(50 mg/L)在20分钟内几乎可被完全去除,60分钟内矿化率分别可达73.7%和91.6%。结合扫描电子显微镜(SEM)、傅里叶变换红外光谱(FT-IR)、X射线衍射(XRD)、X射线光电子能谱(XPS)表征以及电子自旋共振(ESR)检测、电化学分析,探讨了催化体系中的自由基和非自由基途径。石墨化结构和优异的导电性使PSDBC和ZVI@PSDBC不仅在PS活化中作为电子供体产生自由基(主要是SO和·OH),还作为“介质”促进2,4-DCP向催化剂-PS复合物的直接电子转移。PSDBC和ZVI@PSDBC的C=O基团有助于产生O。同时,零价铁纳米颗粒作为PS的反应位点促进了自由基的形成,使得ZVI@PSDBC/PS体系中2,4-DCP降解效果最佳。污泥生物炭材料的稳定性和实用性在可重复使用性和实际废水实验中得到了证明。这些发现为城市污泥的再利用以及废水处理中有效的PS活化提供了一条有前景的途径。

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