Research paperElectrocatalysis degradation of tetracycline in a three-dimensional aeration electrocatalysis reactor (3D-AER) with a flotation-tailings particle electrode (FPE): Physicochemical properties, influencing factors and the degradation mechanism
Graphical Abstract
Introduction
In recent years, antibiotics have been frequently detected in sewage treatment plants (Gurung et al., 2019, Peng et al., 2006), rivers (Zhang et al., 2020) and drinking water (Charuaud et al., 2019). Extrapolating from the latest findings, ascribed antibiotics have a lingering presence in the environment to they do not degrade easily. Antibiotics present in the water environment can lead to the rise of antibiotics resistance genes (ARGs) in humans and animals. Long-term abuse of antibiotics is likely to induce the excretion of ARGs, in animals, causing potential genetic pollution to the surrounding environment (Kairigo et al., 2020). The problem of antibiotic resistance has become one of the global public health safety problems (Abubakar et al., 2020). Particularly widespread use on humans and animals is made of tetracycline (TC), an antibiotic utilized in the treatment of various microbial diseases such as malaria, cholera, bubonic plague, acne, skin and respiratory tract infections (Mosaleheh and Sarvi, 2020, Debnath et al., 2020, Sun et al., 2019). Moreover, TC is unable to completely metabolize in vivo, and therefore large fractions are released into the environment through urine and feces. Therefore, it is urgently important to find an effective remediation process to remove TCs from water.
The existing physical methods, such as coagulation and adsorption, only shift the boundary phase but cannot reduce resistance, while also making the subsequent treatment process more difficult. The biological method leads to the horizontal transmission of resistance genes because of their large biomass, which increases the risk of resistance gene survival. At the same time, TC can reduce the efficiency of the biochemical reaction, have a significantly harmful impact on microorganisms and even lead to the collapse of the bioreactor. Furthermore, although a certain quantity of TC is degraded by microorganisms, the relative abundance of antibiotic resistance genes (ARGs) will also increase (Cheng et al., 2016, Sui et al., 2016). This is due to the proliferation of its host bacteria in the wastewater treatment process or the horizontal transfer of ARGs to other species (Cheng et al., 2016, Subirats et al., 2018). The advanced oxidation process (AOP) is a kind of oxidation reaction with a hydroxyl radical (·OH) as the main active species which has a good mineralization effect on new pollutants such as antibiotics and hormones in the environment. It has a very good degradation effect on TC and has a very high degree of mineralization, thus reducing resistance in the environment. Thanks to this feature, it has attracted the attention of scholars (Wang and Zhuan, 2020).
Electrochemical technology as a type of AOP has made great progress in the treatment of wastewater containing organic pollutants. In fact, electrochemical oxidation provides another solution to many environmental problems in the processing industry, because electrochemical processes are clean, cheap and easy to control, hence their widespread application in environmental pollution control (Ozturk and Yilmaz, 2019, Martínez-Huitle and Panizza, 2018). Furthermore, some researchers developed particle electrodes to be placed between the cathode and anode, and constructed a three-dimensional electrocatalysis system to reduce the mass transfer distance, improve the current efficiency and increase the production of free radicals in the electrocatalysis system (Wu et al., 2019, Zhang et al., 2013). When aeration was added in the electrochemical oxidation reaction, this yielded significant speed advantages (Sun et al., 2017).
According to statistics, 125 tons of tailings are produced for every ton of copper produced (Santander and Valderrama, 2019). Due to the decline in ore grade and process complexity, the production of tailings is increasing year by year. The accumulation of these tailings has brought serious pollution and harm to production and human life, such as environmental and land occupancy hazards as well as the hidden dangers of stacking land. There are also rich and varied chemical elements in flotation tailings, which are of great value in utilization. Therefore, we believe that flotation tailings can give rise to durable electrocatalytic particle electrodes with good mechanical strength, high thermal stability, corrosion resistance and well-developed pore structure under the appropriate proportion and with adequate firing process. In this article, based on the awareness of mineral resource and environmental protection, the particle electrode placed between cathode and anode is made of flotation tailings as well as cheap and simple binders and pore-forming agents, thus greatly reducing its manufacturing cost.
In this study, the main procedures were as follows: I) novel particle electrodes-Flotation-tailings particle electrode (FPE) was prepared using the flotation tailings, garden soil, and soluble starch; II) the physicochemical properties of FPE were characterized by SEM, XRD,FT-IR and XRF methods; III) the adsorption mechanism of tetracycline in solution by FPE was investigated; IV) a three-dimensional aeration electrocatalysis reactor (3D-AER) was constructed and the factors affecting the degradation of tetracycline (TC) and its current efficiency (CE) and current energy consumption (EC) were studied; VI) the kinetics of tetracycline degradation by 3D-AER were analyzed; VII) the action mechanism of·OH in the reaction system was studied by using free radical scavenger tert butyl alcohol (TBA); VIII) the transformation products in water and degradation pathways of Tetracycline was obtained by Ultimate 3000 UHPLC - Q Exactive method.
Section snippets
Chemicals
Tetracycline (TC), NaCl, tert butyl alcohol (TBA) and soluble starch were purchased from Shanghai Aladdin Biochemical Technology Co., Ltd., China. The garden soil comes from the green belt of the University of Jinan. The chemical reagents were used as received. The plexiglass shell was customized in Jinan Jinhui Plexiglass Production Company. The ruthenium iridium-plated titanium mesh was ordered from Jinan Zhuangmeng Co., Ltd.
Preparation of FPE
The primary materials of the flotation-tailings particle electrode
Structural characteristics of FPE
The surface morphologies of FPE were analyzed by SEM technologies. As shown in Fig. 2(a) and (c), the surface and interior of FPE are rough and porous, indicating that FPE possesses numerous, uniform and small pore networks, which can provide extensive active sites and abundant electronic transport pathways, which effectively increases the contact area between sewage and FPE, thus improving the removal rate of TC. Notably, the FPE fault surface (Fig. 2(d)) displays a typical schistose structure
Conclusion
In this study, we carried out several sets of experiments to test the validity of FPE for 3D-AER:
- I)
Preparation of a flotation-tailings particle electrode (FPE): stoving → crushing → proportioning (flotation tailings, garden soil, and soluble starch with a mass ratio of 16:3:1) → blending → ball milling → calcining (1150 ℃) → cooling. Finally FPE was successfully manufactured thanks to these steps. Characterization of FPE: by SEM, XRD, FT-IR and XRF methods, we found that PFE has a high proportion
CRediT authorship contribution statement
Shumin Yang:Conceptualization, Ideas, Methodology, Software, Data curation, Writing - review & editing. Yan Feng: Conceptualization, Ideas, Methodology, Data curation, Supervision, Funding acquisition. Dong Gao: Formal analysis, Data curation. Ning Suo: Investigation, Data curation. Xinwei Wang: Resources, Data curation. Yanzhen Yu: Formal analysis, Data curation. Shoubin Zhang: Resources, Methodology, Data curation, Investigation.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work was funded by a Project of Shandong Province Higher Educational Youth Innovation Science and Technology Program (2020KJG003), the Key Research and Development Plan of Shandong Province (2019GSF109005 and 2017GSF217011), the Natural Science Foundation of Shandong Provincial, China (ZR2017MEE048), the Natural Science Foundation of China (NSFC51678276 and NSFC51608228), the Funding Program of 20 Policies for Universities in Jinan (2018GXRC020). This paper was also supported by the PhD
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