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基于废阳极石墨衍生碳催化剂的合理设计用于激活过一硫酸盐降解莠去津。

Rational design of waste anode graphite-derived carbon catalyst to activate peroxymonosulfate for atrazine degradation.

机构信息

College of Resources and Environmental Engineering, Guizhou University, Guiyang, 550025, PR China.

State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China.

出版信息

Environ Res. 2024 Sep 15;257:119296. doi: 10.1016/j.envres.2024.119296. Epub 2024 May 31.

Abstract

As the rapidly growing number of waste lithium-ion batteries (LIBs), the recycling and reutilization of anode graphite is of increasing interest. Converting waste anode graphite into functional materials may be a sensible option. Herein, a series of carbonaceous catalysts (TG) were successfully prepared using spent anode graphite calcined at various temperatures and applied for activating peroxymonosulfate (PMS) to degrade atrazine (ATZ). The catalyst obtained at 800 °C (TG-800) showed the optimum performance for ATZ removal (99.2% in 6 min). Various experimental conditions were explored to achieve the optimum efficiency of the system. In the TG-800/PMS system, free radicals (e.g., SO, HO·), singlet oxygen (O), together with a direct electron transfer pathway all participated in ATZ degradation, and the ketonic (CO) group was proved as the leading catalytic site for PMS activation. The potential degradation routes of ATZ have also been presented. According to the toxicity assessment experiments, the toxicity of the intermediate products decreased. The reusability and universal applicability of the TG-800 were also confirmed. This research not only provides an efficient PMS activator for pollutant degradation, but also offers a meaningful reference for the recovery of waste anode graphite to develop environmentally functional materials.

摘要

随着废旧锂离子电池(LIB)数量的快速增长,对废旧石墨负极的回收再利用越来越受到关注。将废旧石墨负极转化为功能性材料可能是一个明智的选择。在此,本文使用在不同温度下煅烧的废石墨负极成功制备了一系列碳质催化剂(TG),并将其用于活化过一硫酸盐(PMS)降解莠去津(ATZ)。在 800°C 下煅烧得到的催化剂(TG-800)对 ATZ 的去除效果最佳(6 分钟内去除 99.2%)。本文还探讨了各种实验条件以实现该体系的最佳效率。在 TG-800/PMS 体系中,自由基(如 SO、HO·)、单线态氧(O)以及直接电子转移途径都参与了 ATZ 的降解,酮(CO)基团被证明是 PMS 活化的主要催化位点。此外,还提出了 ATZ 的潜在降解途径。根据毒性评估实验,中间产物的毒性降低。还证实了 TG-800 的可重复使用性和普遍适用性。本研究不仅为污染物降解提供了一种高效的 PMS 活化剂,而且为开发环境功能性材料回收废石墨负极提供了有意义的参考。

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