Jiangxi Water Resources Institute, Nanchang, 330013, Jiangxi Province, China.
School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang, 330013, Jiangxi Province, China.
Environ Sci Pollut Res Int. 2024 Oct;31(49):58999-59011. doi: 10.1007/s11356-024-35167-9. Epub 2024 Sep 27.
In this study, the KOH-modified Fe-ZIF-derived carbon materials (Fe@NC-KOH-x) were designed for Fenton-like systems to enhance bisphenol A (BPA) removal from wastewater. Compared with the Fe@NC without KOH activation, the pore structure, BET (Brunner-Emmet-Teller) surface area, and oxygen-containing functional group of KOH-activated Fe@NC-KOH-x are dramatically improved, which increases the adsorption and catalytic performance. The Fe@NC-KOH-900/PMS system showed significant BPA removal reactivity across wide pH ranges and low doses of Fe@NC-KOH-900. Interestingly, our findings indicated that the removal effectiveness of BPA improved when PMS was introduced following the saturation adsorption of Fe@NC-KOH-x, as compared to the simultaneous introduction of Fe@NC-KOH-x and PMS. More particularly, through regression analysis, we found that the proportion of reactive species in the Fe@NC-KOH-x/PMS system changes with the increase of pyrolysis temperature, and there was a certain relationship between structure-function and active species in the Fe@NC-KOH-x/PMS system. O-C = O, Fe-N, C-O, and pyrrolic N in Fe@NC-KOH-x lead to the generation of •OH, and SO, C = O, Fe-N, and defect are closely related to Fe = O, and the formation of O is affected by Fe-N, graphite N, C = O, and defect. Also, the density functional theory (DFT) calculation and the potential correlation between catalyst active centers and reactive oxygen species indicate that Fe-N is the main active site of Fe@NC-KOH-x. These outcomes of the study offer an innovation for enhanced elimination of BPA in wastewater treatment and provide a dynamic understanding of the mechanism of BPA degradation.
在这项研究中,设计了 KOH 改性的 Fe-ZIF 衍生碳材料(Fe@NC-KOH-x)用于类 Fenton 体系,以增强废水中双酚 A(BPA)的去除。与未经 KOH 活化的 Fe@NC 相比,KOH 活化的 Fe@NC-KOH-x 的孔结构、BET(Brunner-Emmet-Teller)比表面积和含氧官能团得到了显著改善,从而提高了吸附和催化性能。Fe@NC-KOH-900/PMS 体系在很宽的 pH 范围和低剂量的 Fe@NC-KOH-900 下表现出显著的 BPA 去除活性。有趣的是,我们的发现表明,与同时引入 Fe@NC-KOH-x 和 PMS 相比,当 PMS 在 Fe@NC-KOH-x 达到饱和吸附后引入时,BPA 的去除效果会提高。更具体地说,通过回归分析,我们发现 Fe@NC-KOH-x/PMS 体系中活性物质的比例随热解温度的增加而变化,并且在 Fe@NC-KOH-x/PMS 体系中结构-功能和活性物质之间存在一定的关系。Fe@NC-KOH-x 中的 O-C = O、Fe-N、C-O 和吡咯 N 导致 •OH 的产生,SO、C = O、Fe-N 和缺陷与 Fe = O 密切相关,O 的形成受 Fe-N、石墨 N、C = O 和缺陷的影响。此外,密度泛函理论(DFT)计算和催化剂活性中心与活性氧之间的潜在相关性表明,Fe-N 是 Fe@NC-KOH-x 的主要活性位。这项研究的结果为增强废水中 BPA 的去除提供了一种创新方法,并为 BPA 降解机制提供了动态理解。