Please wait a minute...

Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2017, Vol. 11 Issue (2) : 12
The removal of trimethoprim and sulfamethoxazole by a high infiltration rate artificial composite soil treatment system
Qinqin Liu1,2,3,Miao Li3(),Fawang Zhang1,Hechun Yu2,Quan Zhang4,Xiang Liu3()
1. Chinese Academy of Geological Sciences, Beijing 100037, China
2. China University of Geosciences (Beijing), Beijing 100083, China
3. School of Environment, Tsinghua University, Beijing 100084, China
4. Beijing Guohuan Tsinghua Environment Engineering Design & Research Institute Co. Ltd., Beijing 100084, China
Download: PDF(447 KB)   HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Artificial composite soil treatment system with the high infiltration rate (1.394 m·d-1) had a good removal efficiency of TMP (80%–90%) and SMX (60%–70%).

The removal mechanism of TMP and SMX was mainly sorption and was related with hydrogeochemical process.

Sulfamethoxzole (SMX) and trimethoprim (TMP), two combined-using sulfonamide antibiotics, have gained increasing attention in the surface water, groundwater and the drinking water because of the ecological risk. The removal of TMP and SMX by artificial composite soil treatment system (ACST) with different infiltration rates was systematically investigated using K+, Na+, Ca2+, Mg2+ hydrogeochemical indexes. Batch experiments showed that the sorption onto the low-cost and commercially available clay ceramsites was effective for the removal of SMX and TMP from water. The column with more silty clay at high infiltration rate (1.394 m·d1) had removal rates of 80% to 90% for TMP and 60% to 70% for SMX. High SMX and TMP removal rates had a higher effluent concentration of K+, Ca2+ and Mg2+ and had a lower effluent Na+ concentration. Removal was strongly related to sorption. The results showed that the removal of SMX and TMP was related to hydrogeochemical processes. In this study, ACST is determined to be applicable to the drinking water plants.

Keywords Trimethoprim      Sulfamethoxazole      Artificial composite soil treatment      Hydrogeochemical processes      Ion exchange     
Corresponding Authors: Miao Li,Xiang Liu   
Issue Date: 07 April 2017
 Cite this article:   
Qinqin Liu,Miao Li,Fawang Zhang, et al. The removal of trimethoprim and sulfamethoxazole by a high infiltration rate artificial composite soil treatment system[J]. Front. Environ. Sci. Eng., 2017, 11(2): 12.
E-mail this article
E-mail Alert
Articles by authors
Qinqin Liu
Miao Li
Fawang Zhang
Hechun Yu
Quan Zhang
Xiang Liu
chemicals molecular formula CAS# mol. weight water solubility /(mg·L-1 at 25℃) Log Kow pKa1/pKa2
SMX C10H11N3O3S 723-46-6 253.28 410 0.90 1.60/5.70 [21]
TMP C14H18N4O3 738-70-5 290.32 300-400 0.91 3.24/6.76 [21]
Tab.1  The physicochemical properties of SMX, TMP
ASC codes ASC 1 ASC 2 ASC 3 ASC 4
the upper layer Volcanics: silty clay: coarse medium sands v:v:v=2:3:1 Volcanics: silty clay: coarse medium sands v:v:v=5:5:1 silty clay: coarse medium sands v:v=5:1 silty clay: coarse medium sands v:v=2:1
the lower layer clay ceramsites clay ceramsites clay ceramsites clay ceramsites
the supporting of layer cobblestones cobblestones cobblestones cobblestones
CaCl2 deionized solutions
14 d 14 d 14 d 14 d
17-32µg·L1 SMX and TMP deionized solutions 60 d 60 d 60 d 60 d
Tab.2  The experimental scheme of ASC experiment
infiltration rate/(m·d-1) 120.107 183.665 9.346 1.394
the average of porosity 0.291 0.309 0.239 0.246
Tab.3  The average infiltration rates and porosity of four ASCs
Fig.1  Schematic diagram of the ASC
Fig.2  Kinetic study of TMP and SMX sorption onto clay ceramsites. The results were fitted to pseudo-second order kinetic model and the first-order kinetic two-apartment model. (a) Represents the kinetic study of SMX sorption onto clay ceramsites, (b) represents the kinetic study of TMP sorption onto clay ceramsites
fitting parameter pseudo-second order two-apartment
Qe k R2 Qe f k1 k2 R2
SMX 26.839 6.410 0.886 25.541 0.231 6.984 0.060 0.996
TMP 77.331 5.710 0.840 80.967 0.398 2.556 0.053 0.987
Tab.4  Fitting parameter of pseudo-second order kinetic model and the first-order kinetic two-apartment model to the experimental data
Fig.3  Equilibrium data on the sorption of SMX and TMP onto clay ceramsites. The results were fitted to Freundlich, Langmuir and Dubinin-Ashtakhov models. (a) represents the equilibrium study of SMX sorption onto clay ceramsites, (b) represents the equilibrium study of TMP sorption onto clay ceramsites
fitting parameter Freundlich Langmuir DA
n Kf R2 KL Qm R2 Qm E b R2
TMP 0.571 1.661 0.986 0.012 44.981 0.975 151.824 22.247 2.276 0.991
SMX 0.527 0.596 0.980 0.007 23.283 0.985 51.851 22.728 2.721 0.991
Tab.5  Fitting parameter of Frendlich, Langmuir and DA model to the experimental data
Fig.4  The SMX and TMP influent and effluent concentrations variation. (a) represents SMX influent and effluent concentrations variation, (b) represents TMP influent and effluent concentrations variation
Fig.5  The variability of pH and DO over time. (a) Represents pH variability, (b) represents DO variability
Fig.6  The monitoring results of K+, Ca2+, Mg2+ and Na+ concentration over time. (a)-(d) represent K+, Ca2+, Mg2+, and Na+ concentration monitoring result, respectively
1 Fent K, Weston A A, Caminada D. Ecotoxicology of human pharmaceuticals. Aquatic Toxicology (Amsterdam, Netherlands), 2006, 76(2): 122–159
2 Brogden R N, Carmine A A, Heel R C, Speight T M, Avery G S. Trimethoprim: a review of its antibacterial activity, pharmacokinetics and therapeutic use in urinary tract infections. Drugs, 1982, 23(6): 405–430
3 Göbel A, Thomsen A, Mcardell C S, Joss A, Giger W. Occurrence and sorption behavior of sulfonamides, macrolides, and trimethoprim in activated sludge treatment. Environmental Science & Technology, 2005, 39(11): 3981–3989
4 Anquandah G A K, Sharma V K, Knight D A, Batchu S R, Gardinali P R. Oxidation of trimethoprim by ferrate(VI): kinetics, products, and antibacterial activity. Environmental Science & Technology, 2011, 45(24): 10575–10581
5 Ji Y, Xie W, Fan Y, Shi Y, Kong D, Lu J. Degradation of trimethoprim by thermo-activated persulfate oxidation: reaction kinetics and transformation mechanisms. Chemical Engineering Journal, 2016, 286: 16–24
6 Müller E, Schüssler W, Horn H, Lemmer H. Aerobic biodegradation of the sulfonamide antibiotic sulfamethoxazole by activated sludge applied as co-substrate and sole carbon and nitrogen source. Chemosphere, 2013, 92(8): 969–978
7 Reis P J M, Reis A C, Ricken B, Kolvenbach B A, Manaia C M, Corvini P F X, Nunes O C. Biodegradation of sulfamethoxazole and other sulfonamides by Achromobacter denitrificans PR1. Journal of Hazardous Materials, 2014, 280: 741–749
8 Li B, Zhang T. Biodegradation and adsorption of antibiotics in the activated sludge process. Environmental Science & Technology, 2010, 44(9): 3468–3473
9 Kim S H, Shon H K, Ngo H H. Adsorption characteristics of antibiotics trimethoprim on powdered and granular activated carbon. Journal of Industrial and Engineering Chemistry, 2010, 16(3): 344–349
10 Nielsen L, Bandosz T J. Analysis of sulfamethoxazole and trimethoprim adsorption on sewage sludge and fish waste derived adsorbents. Microporous and Mesoporous Materials, 2016, 220: 58–72
11 Koyuncu I, Arikan O A, Wiesner M R, Rice C. Removal of hormones and antibiotics by nanofiltration membranes. Journal of Membrane Science, 2008, 309(1–2): 94–101
12 Radjenović J, Petrović M, Ventura F, Barceló D. Rejection of pharmaceuticals in nanofiltration and reverse osmosis membrane drinking water treatment. Water Research, 2008, 42(14): 3601–3610
13 Dan A, Yang Y, Dai Y, Chen C, Wang S, Tao R. Removal and factors influencing removal of sulfonamides and trimethoprim from domestic sewage in constructed wetlands. Bioresource Technology, 2013, 146: 363–370
14 Choi Y, Kim L, Zoh K. Removal characteristics and mechanism of antibiotics using constructed wetlands. Ecological Engineering, 2016, 91: 85–92
15 Tzanakakis V A, Paranychianakis N V, Angelakis A N. Nutrient removal and biomass production in land treatment systems receiving domestic effluent. Ecological Engineering, 2009, 35(10): 1485–1492
16 Gielen G J H P, Heuvel M R V D, Clinton P W, Greenfield L G. Factors impacting on pharmaceutical leaching following sewage application to land. Chemosphere, 2009, 74(4): 537–542
17 Li L, Lu Z, Wang H, Liu C, Liao R, Zheng F. Experimental study on treatment of polluted river water by constructed rapid infiltration system with new-style combined fillers. China Water & Waste Water. 2007(11): 86–89
18 Wang L, Liu K, Si S, Zhang L, Yan B, Long F. Experimental study of constructed rapid infiltration system with the optimization of combined fillers. Safety and Environmental Engineering. 2013(06): 81–84
19 Back W, Freeze R A. Chemical hydrogeology. American Geophysical Union, 1983
20 Kim J H, Kim R H, Lee J, Chang H W. Hydrogeochemical characterization of major factors affecting the quality of shallow groundwater in the coastal area at Kimje in South Korea. Environmental Geology., 2003, 44(4): 478–489
21 Zarei M, Sedehi F, Raeisi E. Hydrogeochemical characterization of major factors affecting the quality of groundwater in southern Iran, Janah Plain. Chemie der Erde—Geochemistry. 2014, 74(4): 671–680
22 Gao J, Pedersen J A. Adsorption of sulfonamide antimicrobial agents to clay minerals. Environmental Science & Technology, 2005, 39(24): 9509–9516
23 OECD. Guidelines for testing of chemicals test guideline 106: Adsorption- Desorption Using a 380 Batch Equilibrium Method, 2000
24 Wille K, Noppe H, Verheyden K, Vanden Bussche J, De Wulf E, Van Caeter P, Janssen C R, De Brabander H F, Vanhaecke L. Validation and application of an LC-MS/MS method for the simultaneous quantification of 13 pharmaceuticals in seawater. Analytical and Bioanalytical Chemistry, 2010, 397(5): 1797–1808
25 Zhao J, Wang Z, Mashayekhi H, Mayer P, Chefetz B, Xing B. Pulmonary surfactant suppressed phenanthrene adsorption on carbon nanotubes through solubilization and competition as examined by passive dosing technique. Environmental Science & Technology, 2012, 46(10): 5369–5377
26 Essington M E. Soil and Water Chemistry: An Integrative Approach. Boca: CRC Press, 2012
27 Calisto V, Ferreira C I A, Oliveira J A B P, Otero M, Esteves V I. Adsorptive removal of pharmaceuticals from water by commercial and waste-based carbons. Journal of Environmental Management, 2015, 152: 83–90
28 Gu C, Karthikeyan K G. Interaction of tetracycline with aluminum and iron hydrous oxides. Environmental Science & Technology, 2005, 39(8): 2660–2667
29 MacKay A A, Canterbury B. Oxytetracycline sorption to organic matter by metal-bridging. Journal of Environmental Quality, 2005, 34(6): 1964–1971.
30 Jewell K S, Castronovo S, Wick A, Falås P, Joss A, Ternes T A. New insights into the transformation of trimethoprim during biological wastewater treatment. Water Research, 2016, 88: 550–557
[1] FSE-17010-OF-LQQ_suppl_1 Download
Related articles from Frontiers Journals
[1] Qinqin Liu, Miao Li, Xiang Liu, Quan Zhang, Rui Liu, Zhenglu Wang, Xueting Shi, Jin Quan, Xuhui Shen, Fawang Zhang. Removal of sulfamethoxazole and trimethoprim from reclaimed water and the biodegradation mechanism[J]. Front. Environ. Sci. Eng., 2018, 12(6): 6-.
[2] Yi Chen, Shilong He, Mengmeng Zhou, Tingting Pan, Yujia Xu, Yingxin Gao, Hengkang Wang. Feasibility assessment of up-flow anaerobic sludge blanket treatment of sulfamethoxazole pharmaceutical wastewater[J]. Front. Environ. Sci. Eng., 2018, 12(5): 13-.
[3] Ryan C. SMITH,Jinze LI,Surapol PADUNGTHON,Arup K. SENGUPTA. Nexus between polymer support and metal oxide nanoparticles in hybrid nanosorbent materials (HNMs) for sorption/desorption of target ligands[J]. Front. Environ. Sci. Eng., 2015, 9(5): 929-938.
[4] Jing REN,Nan LI,Lin ZHAO,Nanqi REN. Enhanced adsorption of phosphate by loading nanosized ferric oxyhydroxide on anion resin[J]. Front.Environ.Sci.Eng., 2014, 8(4): 531-538.
[5] XIE Bangmi,ZUO Jiane,GAN Lili,LIU Fenglin,WANG Kaijun. Cation exchange resin supported nanoscale zero-valent iron for removal of phosphorus in rainwater runoff[J]. Front.Environ.Sci.Eng., 2014, 8(3): 463-470.
[6] Feng XUE, Beicheng XIA, Rongrong YING, Shili SHEN, Peng ZHAO. Removal of Zn2+ from aqueous solution by biomass of Agaricus bisporus[J]. Front Envir Sci Eng, 2013, 7(4): 531-538.
[7] Qing ZHOU, Mengqiao WANG, Aimin LI, Chendong SHUANG, Mancheng ZHANG, Xiaohan LIU, Liuyan WU. Preparation of a novel anion exchange group modified hyper-crosslinked resin for the effective adsorption of both tetracycline and humic acid[J]. Front Envir Sci Eng, 2013, 7(3): 412-419.
Full text