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蔗糖衍生的 N 掺杂碳干凝胶作为高效过硫酸盐活化剂用于非自由基降解有机污染物。

Sucrose-derived N-doped carbon xerogels as efficient peroxydisulfate activators for non-radical degradation of organic pollutants.

机构信息

School of Environment, Key Laboratory for Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, Henan Normal University, Xinxiang 453007, China.

School of Environment, Key Laboratory for Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, Henan Normal University, Xinxiang 453007, China.

出版信息

J Colloid Interface Sci. 2021 Dec 15;604:660-669. doi: 10.1016/j.jcis.2021.07.019. Epub 2021 Jul 9.

Abstract

Metal-free activation of peroxydisulfate (PDS) for degrading organic pollutants in water has received increasing attention because it can prevent secondary pollution. However, most of the catalysts that are efficient are derived from non-renewable fossil resources, are very expensive and have complex preparation processes. Also, the emerging non-radical mechanism is still unclear. Herein, 3D sucrose-derived N-doped carbon xerogels (NCXs) were synthesized by a simple and sustainable hydrothermal process and then employed as novel metal-free PDS activators to degrade organic pollutants. The structure, composition and performance of NCXs were regulated by changing the carbonization temperature. The sample carbonized at 900 °C (NCX900) exhibited the best catalytic performance, completely removing bisphenol A in 60 min. Quenching experiments and linear sweep voltammograms demonstrated that PDS was activated mainly through an electron-transfer non-radical mechanism. It was found that graphitic N played a critical role in activating PDS. With this non-radical mechanism, the NCX900/PDS system could adapt well to the wide pH range (3-11) and high Cl concentration; it selectively oxidized organic pollutants with low ionization potentials. This work provides a sustainable approach to the low-cost and efficient metal-free catalysts for wastewater treatment.

摘要

无金属活化过一硫酸盐(PDS)用于降解水中的有机污染物受到了越来越多的关注,因为它可以防止二次污染。然而,大多数高效的催化剂都来源于不可再生的化石资源,价格昂贵,且制备过程复杂。此外,新兴的非自由基机制仍不清楚。在此,通过一种简单且可持续的水热工艺合成了 3D 蔗糖衍生的 N 掺杂碳干凝胶(NCXs),并将其用作新型的无金属 PDS 活化剂来降解有机污染物。通过改变碳化温度来调节 NCXs 的结构、组成和性能。在 900°C 碳化的样品(NCX900)表现出最佳的催化性能,在 60 分钟内完全去除双酚 A。猝灭实验和线性扫描伏安法表明,PDS 主要通过电子转移非自由基机制被激活。研究发现,石墨 N 在活化 PDS 中起着关键作用。通过这种非自由基机制,NCX900/PDS 体系能够很好地适应宽 pH 范围(3-11)和高 Cl 浓度;它选择性地氧化具有低电离势的有机污染物。这项工作为废水处理提供了一种可持续的低成本、高效的无金属催化剂的方法。

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