Sustainable design of photo-Fenton-like oxidation process in actual livestock wastewater through the highly dispersed FeCl3 anchoring on a g-C3N4 substrate.

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 FeCl3 on a g-C3N4 substrate (Fe-C3N4) with minimal energy consumption and post-processing. Fe-C3N4 enhances photocatalytic reactivity for antibiotic degradation via a synergistic photo-Fenton-like oxidation technique, efficiently removing antibiotic pollutants from actual livestock wastewater. The Fe-C3N4 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-C3N4Na2SiO3 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-C3N4 catalyst demonstrated high feasibility in treating antibiotic-contaminated livestock wastewater under year-round climatic conditions, leveraging synergistic effects. The stabilization of Fe-C3N4 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-C3N4 and TCHCl, indicating efficient interfacial interactions on the TCHCl surface. To ensure the environmental sustainability of Fe-C3N4, a life cycle assessment (LCA) was conducted to compared this photocatalyst with other commonly used emerging photocatalysts. The results demonstrated that Fe-C3N4 exhibits a two orders of magnitude lower CO2 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.