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用污水污泥和三聚氰胺制备用于过一硫酸盐活化的 N 掺杂生物炭:N 官能团和催化机制。

Preparation of N-doped biochar from sewage sludge and melamine for peroxymonosulfate activation: N-functionality and catalytic mechanisms.

机构信息

CAS Key Laboratory of Crust-Mantle Materials and the Environments, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China; State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, The Chinese Academy of Sciences, Xi'an, Shaanxi 710075, China.

CAS Key Laboratory of Crust-Mantle Materials and the Environments, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China; State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, The Chinese Academy of Sciences, Xi'an, Shaanxi 710075, China.

出版信息

Sci Total Environ. 2020 Nov 20;744:140862. doi: 10.1016/j.scitotenv.2020.140862. Epub 2020 Jul 14.

Abstract

In this study, a group of nitrogen-doped sludge biochar were prepared by a single-step pyrolysis method and employed as catalysts for the activation of peroxymonosulfate (PMS). The N content of as-synthesized biochar composites was altered by adding a different ratio of melamine with the precursors. The sample characterization results indicated that the N content of sludge-melamine-blended biochar named SM-(0.5:1) significantly increased from 1.91 to 9.93% compared with that of raw sludge biochar. Consequently, the surface area and mesoporosity also enhanced. SM-(0.5:1) exhibited excellent degradation ability of reluctant organic pollutants in PMS/acidic media, which outperformed many previously reported carbocatalysts. Complete color removal of a mixture solution of seven cationic and anionic dyes (10 mg L of each) was achieved within 50 min by using 200 mg L of SM-(0.5:1) and 350 mg L of PMS. A mechanism study indicated that the non-radical process performed by the pyridine N dominated the oxidative degradation of pollutants rather than that of SO and OH radical process governed by graphitic N, CO, and surface metal oxides. This study concurrently provides a facile route of enhancing N functionality of sludge-based carbocatalysts and an efficient way of sludge valorization.

摘要

在这项研究中,通过一步热解法制备了一组氮掺杂污泥生物炭,并将其用作过一硫酸盐(PMS)的活化催化剂。通过向原料中添加不同比例的三聚氰胺来改变合成生物炭复合材料的 N 含量。样品表征结果表明,与原始污泥生物炭相比,名为 SM-(0.5:1)的污泥-三聚氰胺混合生物炭的 N 含量从 1.91%显著增加到 9.93%。因此,表面积和中孔也得到了增强。SM-(0.5:1)在 PMS/酸性介质中对难降解有机污染物具有优异的降解能力,优于许多先前报道的碳催化剂。通过使用 200mg/L 的 SM-(0.5:1)和 350mg/L 的 PMS,在 50min 内即可完全去除七种阳离子和阴离子染料(每种 10mg/L)的混合溶液的颜色。机理研究表明,由吡啶 N 主导的非自由基过程支配着污染物的氧化降解,而不是由石墨 N、CO 和表面金属氧化物主导的 SO 和 OH 自由基过程。本研究同时提供了一种增强基于污泥的碳催化剂的 N 功能的简便途径和一种有效的污泥增值方法。

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