{"title":"Biosynthesis of mechanically recyclable 3D-Cu2O@megacatalyst for Fenton-like catalysis of tetracycline and the mechanistic insights","authors":"","doi":"10.1016/j.jece.2024.114191","DOIUrl":null,"url":null,"abstract":"<div><div>Treating sewage waters contaminated with persistent organic pollutants (POPs) presents a pressing environmental concern, mandating, affordable, implementable and sustainable remediations. Supported catalysts, wherein metal nanoparticles are grafted onto inert supports to endow porosity, reactant access, performance and catalyst re-use are emerging as sustainable catalytic platforms. Herein, size-controllable, mechanically recyclable 3D-Cu<sub>2</sub>O@megacatalyst of ∼81 ± 5 cm<sup>2</sup>, ∼37 ± 3 cm<sup>2</sup> and ∼1 ± 0.6 cm<sup>2</sup> were biofabricated by exploiting the innate metal binding feature of pristine eggshells. The as-fabricated Cu<sub>2</sub>O@megacatalyst was utilized for the Fenton-like treatment of POPs, with exceptional activities against diverse molecules: antibiotic (tetracycline (TC)), textile dye (methylene blue) and pharmaceutical precursor (4-nitrophenol) with the degradation efficiencies of 95.6 %, 96.8 % and 93.4 %, respectively. Optimization studies revealed that our megacatalyst can function consistently in the presence of various oxidising agents, free radical scavengers, wide pH, temperatures and inorganic and organic contaminants. The catalyst demonstrated stability and catalytic efficiency in different real-time water matrices: ultrapure water-95.6 %, tap water-84 %, lake water-86 %, and river water-91 %. Furthermore, plausible reaction mechanism and decomposition pathways for TC degradation were assessed using GC-MS, while evaluating the toxicity using ECOSAR and oxygen uptake assay, which revealed less toxic reaction intermediates and end products. Overall, our results provide new insight into the sustainable development of a generalized highly stable, scalable, ultra-efficient and mechanically recyclable Fenton-like supported catalyst for the detoxification of POPs in sewage waters.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343724023224","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Treating sewage waters contaminated with persistent organic pollutants (POPs) presents a pressing environmental concern, mandating, affordable, implementable and sustainable remediations. Supported catalysts, wherein metal nanoparticles are grafted onto inert supports to endow porosity, reactant access, performance and catalyst re-use are emerging as sustainable catalytic platforms. Herein, size-controllable, mechanically recyclable 3D-Cu2O@megacatalyst of ∼81 ± 5 cm2, ∼37 ± 3 cm2 and ∼1 ± 0.6 cm2 were biofabricated by exploiting the innate metal binding feature of pristine eggshells. The as-fabricated Cu2O@megacatalyst was utilized for the Fenton-like treatment of POPs, with exceptional activities against diverse molecules: antibiotic (tetracycline (TC)), textile dye (methylene blue) and pharmaceutical precursor (4-nitrophenol) with the degradation efficiencies of 95.6 %, 96.8 % and 93.4 %, respectively. Optimization studies revealed that our megacatalyst can function consistently in the presence of various oxidising agents, free radical scavengers, wide pH, temperatures and inorganic and organic contaminants. The catalyst demonstrated stability and catalytic efficiency in different real-time water matrices: ultrapure water-95.6 %, tap water-84 %, lake water-86 %, and river water-91 %. Furthermore, plausible reaction mechanism and decomposition pathways for TC degradation were assessed using GC-MS, while evaluating the toxicity using ECOSAR and oxygen uptake assay, which revealed less toxic reaction intermediates and end products. Overall, our results provide new insight into the sustainable development of a generalized highly stable, scalable, ultra-efficient and mechanically recyclable Fenton-like supported catalyst for the detoxification of POPs in sewage waters.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.