Controlling factors of excess sludge on adsorbing trace typical pharmaceuticals

doi:10.11949/j.issn.0438-1157.20170137

Abstract

Abstract:

Conventional biological systems in centralized wastewater treatment plants (WWTPs) are presently inefficient in the removal of pharmaceutical and personal care products (PPCPs), resulting in their ubiquitous presence in excess sludge by absorption. When the sludge is utilized in agricultural land, the absorbed PPCPs may be released and then water environment is contaminated. Therefore, it becomes a crucial issue to predict and assess the content of PPCPs in excess sludge, by revealing the controlling factors of PPCPs adsorption. The adsorption properties of three typical pharmaceuticals onto the sludge from a certain WWTP in Beijing, were investigated based on a trace concentration level using UPLC-MS-MS. The adsorption capacity of ciprofloxacin (CIP) and sulfamethoxazole (SMX) decreased, however, that of acetaminophen (ACP) increased with increasing pH; because the speciation of pharmaceuticals in aqueous solution and zeta potential of biosolid are as a function of pH. Extracellular polymeric substance (EPS) could enhance the adsorption of three typical pharmaceuticals onto the sludge, independent of pH; because the metal ions and organic substances contained in EPS determine the adsorption of pharmaceutical onto the sludge.

Key words: pharmaceutical and personal care products, excess sludge, adsorption, extracellular polymeric substance, metal ion, organic substance

摘要：

传统的污水处理工艺不能完全去除药物和个人护理用品（PPCPs），可能通过吸附作用存在于剩余污泥中。当污泥经土地或农业利用，其中含有的PPCPs可能释放出来，污染水环境，因此，揭示PPCPs经污泥吸附去除的影响因素，对于预测或评估污泥中PPCPs含量尤其重要。以北京某污水处理厂剩余污泥为对象，利用高效液相色谱-质谱联用仪，研究了痕量浓度下3种典型药物在污泥中的赋存特性。随pH增大，环丙沙星与磺胺甲唑的吸附容量减小，而扑热息痛的吸附容量增加；主要是因为pH不仅改变药物在水中的存在形态，而且影响微生物细胞体的表面电位。胞外聚合物（EPS）对污泥吸附3种典型药物均有促进作用，且不依赖于pH；主要是因为EPS中含有的金属离子与有机物成分决定污泥吸附药物性能。

关键词: 药品和个人护理用品, 剩余污泥, 吸附, 胞外聚合物, 金属离子, 有机物

CLC Number:

X523

CAO Daqi, WANG Zhen, HAO Xiaodi, WANG Qunhui. Controlling factors of excess sludge on adsorbing trace typical pharmaceuticals[J]. CIESC Journal, 2017, 68(8): 3266-3274.

曹达啟, 王振, 郝晓地, 汪群慧. 剩余污泥吸附痕量典型药物影响因素[J]. 化工学报, 2017, 68(8): 3266-3274.

References 38

[1]	DAUGHTON C G, TERNES T A. Pharmaceuticals and personal care products in the environment:agents of subtle change?[J]. Environmental Health Perspectives, 1999, 107(Suppl. 6):907-938.
[2]	ALVARINO T, SUAREZ S, KATSOU E, et al. Removal of PPCPs from the sludge supernatant in a one stage nitritation/anammox process[J]. Water Research, 2015, 68:701-709.
[3]	MURRAY K E, THOMAS S M, BODOUR A A. Prioritizing research for trace pollutants and emerging contaminants in the freshwater environment[J]. Environmental Pollution, 2010, 158(12):3462-3471.
[4]	王丹, 隋倩, 赵文涛, 等. 中国地表水环境中药物和个人护理品的研究进展[J]. 科学通报, 2014, 59(9):743-751. WANG D, SUI Q, ZHAO W T, et al. Pharmaceutical and personal care products in the surface water of China:a review[J]. Chinese Science Bulletin, 2014, 59(9):743-751.
[5]	MARTINEZ GOMEZ D A, BACA S, WALSH E J. Lethal and sublethal effects of selected PPCPs on the freshwater rotifer, Plationus patulus[J]. Environmental Toxicology and Chemistry, 2015, 34(4):913-922.
[6]	WANG Z, ZHANG X H, HUANG Y, et al. Comprehensive evaluation of pharmaceuticals and personal care products (PPCPs) in typical highly urbanized regions across China[J]. Environmental Pollution, 2015, 204:223-232.
[7]	BLAIR B, NIKOLAUS A, HEDMAN C, et al. Evaluating the degradation, sorption, and negative mass balances of pharmaceuticals and personal care products during wastewater treatment[J]. Chemosphere, 2015, 134:395-401.
[8]	JOSS A, CARBALLA M, KREUZINGER N, et al. Wastewater treatment//TERNES T A, JOSS A. Human Pharmaceuticals, Hormones and Fragrances:The Challenge of Micropollutants in Urban Water Management[M]. London, UK:IWA Publishing, 2006:243-292.
[9]	KOSMA C I, LAMBROPOULOU D A, ALBANIS T A. Occurrence and removal of PPCPs in municipal and hospital wastewaters in Greece[J]. Journal of Hazardous Materials, 2010, 179(1):804-817.
[10]	GOLET E M, XIFRA I, SIEGRIST H, et al. Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J]. Environmental Science & Technology, 2003, 37(15):3243-3249.
[11]	TERNES T A, HERRMANN N, BONERZ M, et al. A rapid method to measure the solid-water distribution coefficient (Kd) for pharmaceuticals and musk fragrances in sewage sludge[J]. Water Research, 2004, 38(19):4075-4084.
[12]	SUÁREZ S, CARBALLA M, OMIL F, et al. How are pharmaceutical and personal care products (PPCPs) removed from urban wastewaters?[J]. Reviews in Environmental Science and Bio/Technology, 2008, 7(2):125-138.
[13]	RADJENOVI? J, PETROVI? M, BARCELÓ D. Fate and distribution of pharmaceuticals in wastewater and sewage sludge of the conventional activated sludge (CAS) and advanced membrane bioreactor (MBR) treatment[J]. Water Research, 2009, 43(3):831-841.
[14]	MCCLELLAN K, HALDEN R U. Pharmaceuticals and personal care products in archived US biosolids from the 2001 EPA national sewage sludge survey[J]. Water Research, 2010, 44(2):658-668.
[15]	潘寻, 贲伟伟, 强志民. 高效液相色谱-质谱联用法同步测定城市污水处理厂活性污泥中的多类抗生素残留[J]. 分析测试学报, 2011, 30(4):448-452. PAN X, BEN W W, QIANG Z M. Simultaneous determination of several classes of antibiotics in the activated sludge of municipal sewage treatment plants by high performance liquid chromatography-mass spectrometry[J]. Journal of Instrumental Analysis, 2011, 30(4):448-452.
[16]	LIU J L, WONG M H. Pharmaceuticals and personal care products (PPCPs):a review on environmental contamination in China[J]. Environment international, 2013, 59:208-224.
[17]	甘秀梅, 严清, 高旭, 等. 典型抗生素在中国西南地区某污水处理厂中的行为和归趋[J]. 环境科学, 2014, 35(5):1817-1823. GAN X M, YAN Q, GAO X, et al. Occurrence and fate of typical antibiotics in a wastewater treatment plant in Southwest China[J]. Environmental Science, 2014, 35(5):1817-1823.
[18]	URBAIN V, BLOCK J C, MANEM J. Bioflocculation in activated sludge:an analytic approach[J]. Water Research, 1993, 27(5):829-838.
[19]	SHENG G P, YU H Q, LI X Y. Extracellular polymeric substances (EPS) of microbial aggregates in biological wastewater treatment systems:a review[J]. Biotechnology Advances, 2010, 28(6):882-894.
[20]	HA J, GÉLABERT A, SPORMANN A M, et al. Role of extracellular polymeric substances in metal ion complexation on Shewanella oneidensis:batch uptake, thermodynamic modeling, ATR-FTIR, and EXAFS study[J]. Geochimica et Cosmochimica Acta, 2010, 74(1):1-15.
[21]	XU J, SHENG G P, MA Y, et al. Roles of extracellular polymeric substances (EPS) in the migration and removal of sulfamethazine in activated sludge system[J]. Water Research, 2013, 47(14):5298-5306.
[22]	MACKAY A A, CANTERBURY B. Oxytetracycline sorption to organic matter by metal-bridging[J]. Journal of Environmental Quality, 2005, 34(6):1964-1971.
[23]	VASUDEVAN D, BRULAND G L, TORRANCE B S, et al. pH-dependent ciprofloxacin sorption to soils:interaction mechanisms and soil factors influencing sorption[J]. Geoderma, 2009, 151(3):68-76.
[24]	MACKAY A A, VASUDEVAN D. Polyfunctional ionogenic compound sorption:challenges and new approaches to advance predictive models[J]. Environmental Science & Technology, 2012, 46(17):9209-9223.
[25]	POLESEL F, LEHNBERG K, DOTT W, et al. Factors influencing sorption of ciprofloxacin onto activated sludge:experimental assessment and modelling implications[J]. Chemosphere, 2015, 119:105-111.
[26]	YU X Q, ZHANG L P, LIANG M, et al. pH-dependent sulfonamides adsorption by carbon nanotubes with different surface oxygen contents[J]. Chemical Engineering Journal, 2015, 279:363-371.
[27]	BASTOS C A, DE OLIVEIRA M A L. Quantitative determination of acetaminophen, phenylephrine and carbinoxamine in tablets by high-performance liquid chromatography[J]. Química Nova, 2009, 32(7):1951-1955.
[28]	FRØLUND B, PALMGREN R, KEIDING K, et al. Extraction of extracellular polymers from activated sludge using a cation exchange resin[J]. Water Research, 1996, 30(8):1749-1758.
[29]	USEPA. Method 1694:pharmaceuticals and personal care products in water, soil, sediment, and biosolids by HPLC/MS/MS:EPA-821-R-08-002[S]. Washington, DC, 2007.
[30]	CORNELISSEN G, GUSTAFSSON Ö, BUCHELI T D, et al. Extensive sorption of organic compounds to black carbon, coal, and kerogen in sediments and soils:mechanisms and consequences for distribution, bioaccumulation, and biodegradation[J]. Environmental Science & Technology, 2005, 39(18):6881-6895.
[31]	DAHLAN R, MCDONALD C, SUNDERLAND V B. Solubilities and intrinsic dissolution rates of sulfamethoxazole and trimethoprim[J]. Journal of Pharmacy and Pharmacology, 1987, 39(4):246-251.
[32]	CHEN H, GAO B, LI H. Functionalization, pH, and ionic strength influenced sorption of sulfamethoxazole on graphene[J]. Journal of Environmental Chemical Engineering, 2014, 2(1):310-315.
[33]	SCHWARZ J, THIELE-BRUHN S, ECKHARDT K U, et al. Sorption of sulfonamide antibiotics to soil organic sorbents:batch experiments with model compounds and computational chemistry[J]. International Scholarly Research Notices, 2012, 2012(4):1-10.
[34]	URASE T, KIKUTA T. Separate estimation of adsorption and degradation of pharmaceutical substances and estrogens in the activated sludge process[J]. Water Research, 2005, 39(7):1289-1300.
[35]	HÖRSING M, LEDIN A, GRABIC R, et al. Determination of sorption of seventy-five pharmaceuticals in sewage sludge[J]. Water Research, 2011, 45(15):4470-4482.
[36]	WESTERHOFF P, LEE S, YANG Y, et al. Characterization, recovery opportunities, and valuation of metals in municipal sludges from US wastewater treatment plants nationwide[J]. Environmental Science & Technology, 2015, 49(16):9479-9488.
[37]	CARMOSINI N, LEE L S. Ciprofloxacin sorption by dissolved organic carbon from reference and bio-waste materials[J]. Chemosphere, 2009, 77(6):813-820.
[38]	PAN B, QIU M, WU M, et al. The opposite impacts of Cu and Mg cations on dissolved organic matter-ofloxacin interaction[J]. Environmental Pollution, 2012, 161:76-82.

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