Catalytic ozonation of sulfamethoxazole using loaded CuOx/MgO-SiO2 silica aerogel catalyst: Performance, mechanisms and toxicity

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Environmental Research Pub Date : 2025-05-01 Epub Date: 2025-02-20 DOI:10.1016/j.envres.2025.121155
Lanhe Zhang , Jiaming Wu , Jian Zhang , Jingbo Guo
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Abstract

Catalytic ozonation technology can quickly and inexpensively treat antibiotic wastewater, where the performance of catalysts determines the level of catalytic efficiency. In this study, CuOx/MgO-SiO2 (represented by CuMgSiO) catalysts were prepared using hydrothermal method. Their structure and properties were analyzed by X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS) and automatic specific surface area analyzer. The effects of O3 concentration, catalyst dosage and initial pH on the degradation of Sulfamethoxazole (SMX) were investigated. Catalytic ozonation mechanisms and degradation pathways of the pollutants were revealed by quenching experiments and liquid chromatography-mass spectrometry analysis. The toxicity of SMX and its intermediates was analyzed by ECOSAR software. The results showed that CuOx/MgO was successfully loaded onto SiO2 aerogel and the catalyst exhibited a porous network structure. The highest removal efficiency of SMX reached 87.92% and Kobs was 0.07045 min−1 under the optimum conditions, which was 35.9% and 2.77 times higher than those of ozonation alone. The ·OH, ·O2 and 1O2 were active species for the degradation of SMX, and 1O2 played a dominant role. Valence cycling between Cu2+/Cu+ and Mg2+/Mg and adsorption of O3 by surface hydroxyl groups were key steps in catalytic ozonation, and the toxicity of wastewater after treatment was greatly reduced. This study not only provides an economically feasible catalyst, but also offers a new perspective in the field of antibiotic wastewater treatment.

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负载CuOx/MgO-SiO2二氧化硅气凝胶催化剂催化臭氧氧化磺胺甲恶唑:性能、机理和毒性
催化臭氧化技术可以快速、廉价地处理抗生素废水,催化剂的性能决定了催化效率的高低。本研究采用水热法制备CuOx/MgO-SiO2(以CuMgSiO为代表)催化剂。采用x射线衍射仪(XRD)、x射线光电子能谱仪(XPS)和自动比表面积分析仪对其结构和性能进行了分析。考察了O3浓度、催化剂用量和初始pH对磺胺甲恶唑(SMX)降解的影响。通过猝灭实验和液相色谱-质谱分析,揭示了臭氧催化氧化的机理和降解途径。采用ECOSAR软件分析SMX及其中间体的毒性。结果表明:CuOx/MgO被成功负载到SiO2气凝胶上,催化剂呈现多孔网络结构;在此条件下,SMX的最高去除率为87.92%,Kobs为0.07045 min-1,分别比单纯臭氧氧化的去除率高35.9%和2.77倍。·OH、·O2-和1O2是SMX降解的活性物质,其中1O2起主导作用。Cu2+/Cu+和Mg2+/Mg之间的价态循环以及表面羟基对O3的吸附是催化臭氧化的关键步骤,处理后的废水毒性大大降低。本研究不仅提供了一种经济可行的催化剂,而且为抗生素废水处理领域提供了新的视角。
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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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