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嵌入氮掺杂多孔磁性石墨烯中的 FeN 纳米颗粒用于过一硫酸盐活化:自由基和非自由基机制。

FeN nanoparticles embedded in N-doped porous magnetic graphene for peroxymonosulfate activation: Radical and nonradical mechanism.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha, 410082, China.

School of Architecture and Art, Central South University, Changsha, 410083, China.

出版信息

Chemosphere. 2022 Oct;305:135317. doi: 10.1016/j.chemosphere.2022.135317. Epub 2022 Jun 13.

Abstract

The persistence of pharmaceutical and personal care products (PPCPs) such as norfloxacin (NFX) poses a serious threat to the water environment, and the development of efficient and cost-effective advanced oxidation catalysts is an important step toward resolving this issue. Herein, Fe and N co-doped graphene (FeNGO) was synthesized from graphene oxide (GO), urea, and iron salt via simple impregnation pyrolysis, and applied for activating peroxymonosulfate (PMS) to degrade NFX. FeNGO possessed a two-dimensional porous sheet structure and was rich in defects, nitrogen species, and active sites. Compared with the control catalyst doped with N or Fe alone, FeNGO/PMS system showed the best degradation performance with 97.7% removal of NFX after 30 min, the rate constant was 7.1 and 1.7 times than that for NGO and FeGO, respectively. FeN was the main active site of FeNGO, and it is confirmed that singlet oxygen (O) and superoxide radical (O) were the primary oxidation active species (ROS) during NFX degradation. The formation of O came from the transformation of O and PMS decomposition. FeNGO showed strong pH adaptability, and also exhibited stale degradation performance in saliferous water matrices. It is believed that this work will offer theoretical and practical guidance for PMS activation by non-radical pathways.

摘要

药物和个人护理产品(PPCPs)如诺氟沙星(NFX)的持久性对水环境构成了严重威胁,开发高效且具有成本效益的高级氧化催化剂是解决这一问题的重要步骤。本文通过简单的浸渍热解,由氧化石墨烯(GO)、尿素和铁盐合成了 Fe 和 N 共掺杂石墨烯(FeNGO),并将其用于激活过一硫酸盐(PMS)来降解 NFX。FeNGO 具有二维多孔片层结构,富含缺陷、氮物种和活性位点。与单独掺杂 N 或 Fe 的对照催化剂相比,FeNGO/PMS 体系在 30 分钟内表现出最好的 NFX 去除效果,去除率为 97.7%,其速率常数分别是 NGO 和 FeGO 的 7.1 和 1.7 倍。FeN 是 FeNGO 的主要活性位点,并且证实 singlet oxygen (O) 和 superoxide radical (O) 是 NFX 降解过程中的主要氧化活性物质(ROS)。O 的形成来自于 O 和 PMS 分解的转化。FeNGO 表现出很强的 pH 适应性,在含盐水体基质中也表现出稳定的降解性能。相信这项工作将为非自由基途径激活 PMS 提供理论和实践指导。

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