School of Environment, Key Laboratory for Yellow River and Huai River Water Environmental and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, Henan Normal University, Xinxiang, Henan, 453007, PR China; Institute of Chemistry, Henan Academy of Sciences, Zhengzhou, Henan, 450002, PR China.
School of Environment, Key Laboratory for Yellow River and Huai River Water Environmental and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, Henan Normal University, Xinxiang, Henan, 453007, PR China.
Chemosphere. 2023 Jan;311(Pt 1):137022. doi: 10.1016/j.chemosphere.2022.137022. Epub 2022 Oct 29.
N-doped carbons have attracted extensive attention as catalysts for peroxymonosulfate (PMS) activation towards environmental remediation. However, synthesis of N-rich carbocatalysts is challenging and PMS activation mechanism is still unclear. Herein, novel N-rich porous carbocatalysts (C-PCN-T) were synthesized by carbonization of polyaniline nanorods coated g-CN. C-PCN-900 (polyaniline content 50%) calcined at 900 °C had high surface area (358 m/g), product yield (27.1%) and N content (12.27 at%). It showed superior performance in activating PMS to degrade and mineralize various phenolic pollutants in a wide pH range (2-11) and with the co-existence of water constituents. A positive correlation was observed between phenol oxidation rates and contents of CO, C-C/CC and graphitic N, which served as active sites to facilitate adsorption of pollutants and PMS on C-PCN-900 and subsequent electron-transfer from pollutants to PMS. Overall, this study provides new insights into rational design of N-doped carbocatalysts and elucidation of electron transfer pathway in PMS activation.
氮掺杂碳作为过一硫酸盐 (PMS) 活化催化剂在环境修复中受到广泛关注。然而，富氮碳催化剂的合成具有挑战性，且 PMS 活化机制尚不清楚。本文通过苯胺纳米棒包覆 g-CN 的碳化合成了新型富氮多孔碳催化剂 (C-PCN-T)。在 900°C 下煅烧的含 50%苯胺的 C-PCN-900 具有高比表面积（358 m/g）、产率（27.1%）和氮含量（12.27%）。它在活化 PMS 以降解和矿化各种酚类污染物方面表现出优异的性能，适用的 pH 值范围广（2-11），且在水成分共存的情况下仍具有良好的效果。酚类氧化速率与 CO、C-C/CC 和石墨化 N 的含量呈正相关，这些物质作为活性位点，有利于污染物和 PMS 在 C-PCN-900 上的吸附，以及随后污染物向 PMS 的电子转移。总的来说，本研究为合理设计氮掺杂碳催化剂和阐明 PMS 活化中的电子转移途径提供了新的思路。
