Chlortetracycline removal by using hydrogen based membrane biofilm reactor

doi:10.1016/j.jhazmat.2016.08.014

Journal of Hazardous Materials

Volume 320, 15 December 2016, Pages 88-95

https://doi.org/10.1016/j.jhazmat.2016.08.014 Get rights and content

Highlights

•
H₂-MBfR accomplished the simultaneous removal of nitrate and chlortetracycline.
•
H₂-MBfR provides an appropriate environment to degrade CTC under anoxic conditions.
•
Transformation products were ECTC, ACTC and EACTC formed at ppt levels.
•
Betaproteobacteria was the most responsible microbial family in the CTC biodegradation.

Abstract

In the last years, increasing attention has been paid on the presence of antibiotics in aqueous environments due to their ecological damage and potential adverse effects on organisms. Membrane biofilm reactors (MBfR) have been gained a significant popularity as an advanced wastewater treatment technology in removing of organic micro-pollutants. In this study, the performance of H₂-MBfR for simultaneous removal of nitrate and chlortetracycline, formation of transformation products and community analysis of the biofilm grown on the gas permeable hollow fiber membranes was evaluated by considering effect of the hydraulic retention time, surface loadings of target pollutants and H₂ pressure. The results showed that the simultaneous chlortetracycline (96%) and nitrate removal (99%) took placed successfully under the conditions of 5 h HRT and 2 psi H₂ pressure. It has been determined that the main elimination process was biodegradation and Betaproteobacteria species was responsible for chlortetracycline degradation.

Introduction

Over the past few years, antibiotics have been considered emerging pollutants due to their continuous input and persistence in the aquatic ecosystem even at low concentrations. Although most of the antibiotics are used for the treatment of infections in humans and animals, a significant portion of the most antibiotics is also used in feed as a supplement to promote animal growth.

Antibiotics can enter the environment through a number of routes such as including the drug manufacturing process and disposal of unused drugs and containers [1]. Moreover, the ratio of 30–90% of their used amount are excreted into the waste system because most of the antibiotics are not completely metabolized or eliminated in the body [2]. As a result of their widespread use, antibiotics release into the environment and they are considered to be emerging pollutants due to their bioactivity, polarity and persistence which may cause adverse effects on aquatic life and humans [3]. Antibiotics may lead to the emergence of new strains of bacteria that are resistant to these antibiotics and, in turn, result in untreatable livestock diseases. A potentially more dangerous scenario is the possible transmission of such strains to humans, resulting in untreatable human diseases [4]. Drinking water in areas with growing urban populations is commonly supplied from surface water sources. Thus, it is an important approach to develop the acceptable methods in effectively removing the antibiotics in aqueous environments.

Recently, extensive researches have been carried out on the degradation and removal of the antibiotics from aqueous systems by advanced oxidation proceses [5], photocatalysis [6], [7], [8], sonocatalysis [9], chlorination [10], sorption [11], [12], [13], reverse osmosis [14], activated sludge process [12], [15], [16] and membrane biorectors (MBRs) [3], [17], [18], [19], [20]. Among the processes mentioned above, biological treatment methods have been interested because of the quantity of energy and chemical reagents consumed during the AOPs. It is reported that conventional biological processes are insufficient to degrade and mineralize the antibiotics [16]. Particularly, the hydrogen-based membrane biofilm reactor (H₂-MBfR) is a new technology to reduce many contaminants from water. Many researchers reported that the H₂-MBfR could simultaneously reduce multiple oxidized contaminants by using H₂ gas substrate as the universal electron donor [21], [22], [23]. In these systems, H₂ is considered as the electron donor for bio-reduction, because H₂ is non-toxic, leaves no residuals that could cause bacterial re-growth, is relatively inexpensive, and is a biologically available electron donor for the reduction of many oxidized contaminants.

The main goals of the present study were i) to investigate chlortetracycline bioreduction and to evaluate the feasibility of the H₂-MBfR in improving the removal efficiency of the chlortetracycline from aqueous solutions, ii) to investigate the qualitative and quantitative monitoring of the transformation products of chlortetracycline, and iii) to define changes in microbial population in biofilm.

Section snippets

H₂ based membrane biofilm reactor

Membrane biofilm reactor (MBfR) used in the study consisted of two glass tubes including membrane module. The main membrane module included 40 hydrophobic hollow fiber gas transfer membrane in the glass tube and other was sampling column including a few fibers for biofilm samples (Fig. 1). Since the membrane modules located in both glass tubes were fed with H₂ gas as electron donor, the system was named as Hydrogen based Membrane Biofilm Reactor (H₂-MBfR). The total surface area of gas transfer

H₂-MBfR performance for denitrification and CTC removal

In order to evaluate the simultaneous denitrification and antibiotic removal by H₂ based MBfR, we operated the system under different HRTs and H₂ gas pressures. The results demonstrated that H₂-MBfR concept could be successfully applied to treat the water bodies including the oxidized contaminants and CTC. Fig. 2 indicates the average efficiencies of both nitrate and CTC removals at each HRT and gas pressure. During P1 (HRT = 15 h), the system achieved efficiency of both denitrification and CTC

Conclusions

The performance of the H₂-MBfR for removal of chlortetracycline from aqueous solutions, and concerning the mechanisms and microbial community responsible for the removal of target molecule in the H₂-MBfR were investigated in this study. The system accomplished successfully the simultaneous denitrification and chlortetracycline removal. Almost complete denitrification and higher than 96% chlortetracycline removal were achieved at the conditions of H₂ pressure of 2 and 5 h of HRT. It was found

Acknowledgement

A significant part of this paper includes Master Thesis data of Ekrem Aydın. Authors graceful acknowledge the financial support from The Scientific and Technological Research Council of Turkey (TUBITAK) with the project number of 112Y261. In addition, they would like to remind the projects of TUBITAK-108Y136 using PCR and DGGE equipment for molecular studies, TUBITAK-111Y092 using HPLC for CTC analyses, and FUBAP-1736 using LC–MS/MS for CTC by-products. However, authors thank Expert Mehmet

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Chlortetracycline removal by using hydrogen based membrane biofilm reactor

Highlights

Abstract

Introduction

Section snippets

H2 based membrane biofilm reactor

H2-MBfR performance for denitrification and CTC removal

Conclusions

Acknowledgement

J. Environ. Manag.

Sci. Total Environ.

Bioresour. Technol.

Sol. Energy

Water Res.

Process Biochem.

J. Hazard. Mater.

Sep. Purif. Technol.

Water Res.

Water Res.

Desalination

Bioresour. Technol.

Bioresour. Technol.

Water Res.

Water Res.

Bioresour. Technol.

J. Environ. Sci.

Appl. Clay Sci.

Water Res.

J. Biol. Chem.

H₂ based membrane biofilm reactor

H₂-MBfR performance for denitrification and CTC removal