College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.
Key Laboratory of Water Pollution Control Technology, Hunan Research Academy of Environmental Sciences, Changsha 410004, PR China.
J Colloid Interface Sci. 2021 Mar 15;586:551-562. doi: 10.1016/j.jcis.2020.10.120. Epub 2020 Oct 29.
A novel in-situ N-doped carbon nanoparticles (NCNs) was prepared through direct pyrolysis of N-rich polyaniline (PANI) without using external N-containing precursor and the as-prepared materials were employed as metal-free peroxydisulfate (PDS) activator for bisphenol A (BPA) degradation. The catalyst derived from PANI carbonization at 900 °C (NCNs-9) displayed the excellent catalytic activity to activate PDS, resulting in 96.0% BPA degradation efficiency within 20 min. The catalytic activity of NCNs was closely related to their structure-composition, and higher graphitic N content and larger BET surface area were beneficial to the generation of reactive oxygen species (ROS). The quenching tests and electron paramagnetic resonance (EPR) demonstrated that BPA degradation in PDS/NCNs system was accomplished via non-radical (O) and radical ( ·OH, SO·, and O·) pathways, in which O· was the main ROS. The origin of O· was the conversion of dissolved oxygen and the activation of PDS. The possible degradation pathways of BPA were also proposed. This study might provide inspirations to design in-situ N-doped carbon nanoparticles as the PDS activator for efficient degradation of persistent organic compound via advanced oxidation processes (AOPs).
一种新型的原位 N 掺杂碳纳米粒子(NCNs)是通过直接热解富氮聚苯胺(PANI)制备的,无需使用外部含 N 前体,所制备的材料被用作无金属过二硫酸盐(PDS)活化剂用于双酚 A(BPA)降解。在 900°C 下碳化 PANI 得到的催化剂(NCNs-9)对 PDS 的活化具有优异的催化活性,在 20 分钟内可实现 96.0%的 BPA 降解效率。NCNs 的催化活性与其结构-组成密切相关,较高的石墨 N 含量和较大的 BET 表面积有利于活性氧物种(ROS)的生成。淬灭实验和电子顺磁共振(EPR)表明,在 PDS/NCNs 体系中,BPA 降解是通过非自由基(O)和自由基(·OH、SO·和 O·)途径完成的,其中 O·是主要的 ROS。O·的来源是溶解氧的转化和 PDS 的活化。还提出了 BPA 的可能降解途径。这项研究可能为设计原位 N 掺杂碳纳米粒子作为 PDS 活化剂,通过高级氧化工艺(AOPs)有效降解持久性有机化合物提供启示。