College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.
College of Environmental Science and Engineering, Hunan University, Changsha, Hunan 410082, China; Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, Hunan 410082, China.
J Hazard Mater. 2023 Jan 5;441:129895. doi: 10.1016/j.jhazmat.2022.129895. Epub 2022 Sep 3.
In this study, a graphene shell-encapsulated copper-based nanoparticles (G@Cu-NPs) was prepared and employed for peracetic acid (PAA) activation. The characterization of G@Cu-NPs confirmed that the as-prepared material was composed of Cu and CuO inside and encapsulated by a graphene shell. Experimental results suggested that the synthesized G@Cu-NPs could activate PAA to generate free radicals for efficiently removing sulfamethazine (SMT) under neutral condition. The formation of graphene shells could strongly facilitated electron transfer from the core to the surface. Radical quenching experiments and electron spin resonance (ESR) analysis confirmed that organic radicals (R-O•) and hydroxyl radicals (•OH) were generated in the G@Cu-NPs/PAA system, and R-O• (including CHCO• and CHCO•) was the main contributor to the elimination of SMT. The possible SMT degradation pathways and mechanisms were proposed, and the toxicity of SMT and its intermediates was predicted with the quantitative structure-activity relationship (QSAR) analysis. Besides, the effects of some key parameters, common anions, and humic acid (HA) on the removal of SMT in the G@Cu-NPs/PAA system were also investigated. Finally, the applicability of G@Cu-NPs/PAA system was explored, showing that the G@Cu-NPs/PAA system possessed satisfactory adaptability to treat different water bodies with admirable reusability and stability.
在这项研究中，制备了一种石墨烯壳包裹的铜基纳米粒子（G@Cu-NPs），并将其用于过乙酸（PAA）活化。G@Cu-NPs 的表征证实，所制备的材料由内部的 Cu 和 CuO 以及外部的石墨烯壳组成。实验结果表明，所合成的 G@Cu-NPs 可以在中性条件下激活 PAA 生成自由基，从而有效地去除磺胺甲噁唑（SMT）。石墨烯壳的形成可以强烈促进电子从核心向表面转移。自由基猝灭实验和电子自旋共振（ESR）分析证实，在 G@Cu-NPs/PAA 体系中生成了有机自由基（R-O•）和羟基自由基（•OH），而 R-O•（包括 CHCO•和 CHCO•）是去除 SMT 的主要贡献者。提出了可能的 SMT 降解途径和机制，并通过定量结构-活性关系（QSAR）分析预测了 SMT 及其中间产物的毒性。此外，还研究了一些关键参数、常见阴离子和腐殖酸（HA）对 G@Cu-NPs/PAA 体系中 SMT 去除的影响。最后，还探索了 G@Cu-NPs/PAA 体系的适用性，结果表明，G@Cu-NPs/PAA 体系对处理不同水体具有令人满意的适应性，具有良好的可重复使用性和稳定性。
