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通过将高分散的 FeCl 锚定在 g-CN 基底上来实现实际养殖废水中类芬顿光氧化过程的可持续设计。

Sustainable design of photo-Fenton-like oxidation process in actual livestock wastewater through the highly dispersed FeCl anchoring on a g-CN substrate.

机构信息

Key Laboratory of Agro-Environment in Downstream of Yangtze Plain, Ministry of Agriculture and Rural Affairs, Institute of Agricultural Resources and Environment, Jiangsu Academy of Agricultural Sciences, Nanjing 210014, China.

Key Laboratory of Agro-Environment in Downstream of Yangtze Plain, Ministry of Agriculture and Rural Affairs, Institute of Agricultural Resources and Environment, Jiangsu Academy of Agricultural Sciences, Nanjing 210014, China; Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China.

出版信息

Water Res. 2024 Aug 1;259:121889. doi: 10.1016/j.watres.2024.121889. Epub 2024 Jun 4.

Abstract

Photocatalytic technology emerges as a promising solution for the sustainable treatment of contaminated wastewater. However, the practical implementation of designed photocatalysts often faces challenges due to the intricate 'high carbon footprint' process and limited outdoor laboratory investigations. Herein, a simple yet versatile impregnation approach is proposed to anchor highly dispersed FeCl on a g-CN substrate (Fe-CN) with minimal energy consumption and post-processing. Fe-CN enhances photocatalytic reactivity for antibiotic degradation via a synergistic photo-Fenton-like oxidation technique, efficiently removing antibiotic pollutants from actual livestock wastewater. The Fe-CN catalyst exhibited consistent degradation performance over five cycles in laboratory conditions, maintaining a degradation efficiency exceeding 90 % for tetracycline hydrochloride (TCHCl). Furthermore, we engineered a straightforward Fe-CNNaSiO reactor for treating livestock wastewater, achieving an 81.8 % removal of TCHCl in outdoor field tests conducted in the winter and summer in China. The Fe-CN catalyst demonstrated high feasibility in treating antibiotic-contaminated livestock wastewater under year-round climatic conditions, leveraging synergistic effects. The stabilization of Fe-CN for the degradation of antibiotic-containing wastewater under sunlight represents a significant advancement in the practical application of photocatalysts, marking a crucial milestone from experimental conception to implementation. Acute toxicity estimation suggested that intermediates/products generated exhibited lower toxicity compared to TCHCl, indicating their practical applicability. Density functional theory (DFT) analysis successfully predicted significant electron transfer between Fe-CN and TCHCl, indicating efficient interfacial interactions on the TCHCl surface. To ensure the environmental sustainability of Fe-CN, a life cycle assessment (LCA) was conducted to compared this photocatalyst with other commonly used emerging photocatalysts. The results demonstrated that Fe-CN exhibits a two orders of magnitude lower CO equivalent emission compared to the ZnO photocatalyst, indicating a cost-effective and efficient synergistic photo-Fenton-like catalytic approach. This low-cost photocatalyst, moving from the laboratory to real-world wastewater applications, provides a powerful and more sustainable solution for the efficient treatment of wastewater containing antibiotics from livestock farming.

摘要

光催化技术作为一种可持续处理受污染废水的有前途的解决方案而出现。然而,由于复杂的“高碳足迹”过程和有限的户外实验室研究,设计的光催化剂的实际实施常常面临挑战。在此,提出了一种简单而通用的浸渍方法,以最小的能量消耗和后处理将高度分散的 FeCl 锚定在 g-CN 基底上(Fe-CN)。Fe-CN 通过协同光芬顿样氧化技术增强了抗生素降解的光催化反应性,有效地从实际的牲畜废水中去除抗生素污染物。在实验室条件下,Fe-CN 催化剂在五个循环中表现出一致的降解性能,保持盐酸四环素(TCHCl)的降解效率超过 90%。此外,我们设计了一种简单的 Fe-CNNaSiO 反应器来处理牲畜废水,在中国的冬季和夏季户外现场测试中实现了 TCHCl 去除率达到 81.8%。Fe-CN 催化剂在全年气候条件下处理含抗生素的牲畜废水方面表现出很高的可行性,利用协同效应。Fe-CN 用于在阳光下降解含抗生素废水的稳定性代表了光催化剂实际应用的重大进展,标志着从实验构思到实施的重要里程碑。急性毒性评估表明,与 TCHCl 相比,生成的中间体/产物表现出较低的毒性,表明其实际适用性。密度泛函理论(DFT)分析成功预测了 Fe-CN 和 TCHCl 之间的显著电子转移,表明在 TCHCl 表面存在有效的界面相互作用。为了确保 Fe-CN 的环境可持续性,进行了生命周期评估(LCA),将这种光催化剂与其他常用的新兴光催化剂进行了比较。结果表明,与 ZnO 光催化剂相比,Fe-CN 的 CO 当量排放低两个数量级,表明这是一种具有成本效益且高效的协同光芬顿样催化方法。这种低成本的光催化剂从实验室转移到实际的废水应用中,为高效处理来自畜牧业的含抗生素废水提供了一种强大且更可持续的解决方案。

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