Please wait a minute...

Frontiers of Environmental Science & Engineering

Front Envir Sci Eng    2012, Vol. 6 Issue (6) : 784-796
Fluorescence spectroscopic studies of the effect of granular activated carbon adsorption on structural properties of dissolved organic matter fractions
Shuang XUE1,2, Qingliang ZHAO3, Liangliang WEI3, Xiujuan HUI1,2(), Xiping MA1,2, Yingzi LIN4
1. School of Environmental Science, Liaoning University, Shenyang 110036, China; 2. Key Laboratory of Water Environment Biomonitoring and Ecological Security Liaoning Province, Shenyang 110036, China; 3. School of Municipal & Environmental Engineering, Harbin Institute of Technology, Harbin 150090, China; 4. Key Laboratory of Songliao Aquatic Environment, Ministry of Education, Jilin Architectural and Civil Engineering Institute, Changchun 130118, China
Download: PDF(753 KB)   HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

This work investigated the effect of granular activated carbon adsorption (GACA) on fluorescence characteristics of dissolved organic matter (DOM) in secondary effluent, by means of excitation–emission matrix (EEM) spectra, the fluorescence regional integration (FRI) method, synchronous spectra, the fluorescence index defined as the ratio of fluorescence emission intensity at wavelength 450 nm to that at 500 nm at excitation (λex)=370 nm, and the wavelength that corresponds to the position of the normalized emission band at its half intensity (λ0.5). DOM in the secondary effluent from the North Wastewater Treatment Plant (Shenyang, China) was fractionated using XAD resins into 5 fractions: hydrophobic acid (HPO–A), hydrophobic neutral (HPO–N), transphilic acid (TPI–A), transphilic neutral (TPI–N) and hydrophilic fraction (HPI). Results showed that fluorescent materials in HPO–N and TPI–N were less readily removed than those in the other fractions by GACA. The relative content of fluorescent materials in HPO–A, TPI–A and HPI decreased whereas that in HPO–N and TPI–N increased as a consequence of GACA. Polycyclic aromatics in all DOM fractions were preferentially absorbed by GACA, in comparison with bulk DOM expressed as DOC. On the other hand, the adsorption of aromatic amino acids and humic acid-like fluorophores exhibiting fluorescence peaks in synchronous spectra by GACA seemed to be dependent on the acid/neutral properties of DOM fractions. All five fractions had decreased fluorescence indices as a result of GACA. GACA led to a decreased λ0.5 value for HPO–A, increased λ0.5 values for HPO–N, TPI–A and HPI, and a consistent λ0.5 value for TPI–N.

Keywords granular activated carbon adsorption      dissolved organic matter      fractionation      fluorescence     
Corresponding Authors: HUI Xiujuan,   
Issue Date: 01 December 2012
 Cite this article:   
Shuang XUE,Qingliang ZHAO,Liangliang WEI, et al. Fluorescence spectroscopic studies of the effect of granular activated carbon adsorption on structural properties of dissolved organic matter fractions[J]. Front Envir Sci Eng, 2012, 6(6): 784-796.
E-mail this article
E-mail Alert
Articles by authors
Shuang XUE
Qingliang ZHAO
Liangliang WEI
Xiujuan HUI
Xiping MA
Yingzi LIN
pH8.1Br-(μg·L-1)<20 a)
TOC (mg·L-1)17.3Ammonia (mg N·L-1)5.3
DOC (mg·L-1)13.7Nitrate (mg N·L-1)13.9
UV–254 (m-1)18.7Alkalinity (mg CaCO3·L-1)105.8
Tab.1  Characteristics of the NWTP secondary effluent
Fig.1  XAD fractionation of DOM before and after GACA. The two pie diagrams indicate the distributions of five DOM fractions in the water samples
Fig.2  EEM spectra of DOM fractions before and after GACA
DOM fractionΦI+ II, n ( × 10-7)/(AU·nm2·mg·L-1)ΦIII, n ( × 10-7)/(AU·nm2·mg·L-1)ΦIV, n ( × 10-7)/(AU·nm2·mg·L-1)ΦV, n ( × 10-7)/((AU·nm2·mg·L-1)ΦT, n ( × 10-7)/(AU·nm2·mg·L-1)PI+ II, n/%PIII, n/%PIV, n/%PV, n/%
before GACA
after GACA
Tab.2  , and values for DOM fractions before and after GACA
Fig.3  Total (a), total (b), total (c), total (d) and total (e) value for DOM fractions before and after GACA
HPO–A, HPO–N, TPI–A, TPI–N and HPI accounted for 37%, 10%, 20%, 19% and 14% of fluorescence in the NWTP secondary effluent (Fig. 4). With the high value, HPO–A, TPI–A and TPI–N contributed more to fluorescence than they contributed to DOC, and this was contrary to HPO–N and HPI. The contribution of HPO–A, TPI–A and HPI to fluorescence decreased after GACA, due to preferential removal of fluorescent materials in these three fractions during GACA. In contrast, the contribution of HPO–N and TPI–N increased. As a result, TPI–N became the major contributor and was responsible for 33% of the fluorescence after GACA. HPO–A ranked second, constituting 30% of the fluorescence after GACA. HPO–N, TPI–A and HPI were relatively unimportant, corresponding to 13%, 13% and 11% of the fluorescence after GACA.
Fig.4  Contributions DOM fractions to fluorescence before and after GACA
Fig.5  synchronous spectra of DOM fractions with ? = 18 nm (a) and with ? = 66 nm (b) before and after GACA
Fig.6  Fluorescence emission spectra of DOM fractions at = 370 nm before and after GACA
Fig.7  in the normalized fluorescence emission spectra of DOM fractions before and after GACA
1 Ryu H, Alum A, Abbaszadegan M. Microbial characterization and population changes in nonpotable reclaimed water distribution systems. Environmental Science & Technology , 2005, 39(22): 8600-8605
doi: 10.1021/es050607l pmid:16323753
2 Matamoros V, Mujeriego R, Bayona J M. Trihalomethane occurrence in chlorinated reclaimed water at full-scale wastewater treatment plants in NE Spain. Water Research , 2007, 41(15): 3337-3344
doi: 10.1016/j.watres.2007.04.021 pmid:17585988
3 Cloirec P L, Brasquet C, Subrenat E. Adsorptiononto fibrous activated carbon: applications to water treatment. Energy & Fuels , 1997, 11(2): 331-336
doi: 10.1021/ef9601430
4 Karanfil T, Kitis M, Kilduff J E, Wigton A. Role of granular activated carbon surface chemistry on the adsorption of organic compounds. 2. Natural organic matter. Environmental Science & Technology , 1999, 33(18): 3225-3233
doi: 10.1021/es9810179
5 Vahala R, Langvik V A, Laukkanen R. Controlling adsorbable organic halogens (AOX) and trihalomethanes (THM) formation by ozonation and two-step granule activated carbon (GAC) filtration. Water Science and Technology , 1999, 40(9): 249-256
doi: 10.1016/S0273–1223(99)00663–0
6 Uyak V, Yavuz S, Toroz I, Ozaydin S, Genceli E A. Disinfection by-products precursors removal by enhanced coagulation and PAC adsorption. Desalination , 2007, 216(1-3): 334-344
doi: 10.1016/j.desal.2006.11.026
7 Humbert H, Gallard H, Suty H, Croué J P. Natural organic matter (NOM) and pesticides removal using a combination of ion exchange resin and powdered activated carbon (PAC). Water Research , 2008, 42(6-7): 1635-1643
doi: 10.1016/j.watres.2007.10.012 pmid:18006038
8 Cheng W, Dastgheib S A, Karanfil T. Adsorption of dissolved natural organic matter by modified activated carbons. Water Research , 2005, 39(11): 2281-2290
doi: 10.1016/j.watres.2005.01.031 pmid:15927230
9 Quinlivan P A, Li L, Knappe D R U. Effects of activated carbon characteristics on the simultaneous adsorption of aqueous organic micropollutants and natural organic matter. Water Research , 2005, 39(8): 1663-1673
doi: 10.1016/j.watres.2005.01.029 pmid:15878039
10 Schreiber B, Brinkmann T, Schmalz V, Worch E. Adsorption of dissolved organic matter onto activated carbon—the influence of temperature, absorption wavelength, and molecular size. Water Research , 2005, 39(15): 3449-3456
doi: 10.1016/j.watres.2005.05.050 pmid:16055163
11 Haberkamp J, Ruhl A S, Ernst M, Jekel M. Impact of coagulation and adsorption on DOC fractions of secondary effluent and resulting fouling behaviour in ultrafiltration. Water Research , 2007, 41(17): 3794-3802
doi: 10.1016/j.watres.2007.05.029 pmid:17585987
12 Wei L L, Zhao Q L, Xue S, Jia T. Removal and transformation of dissolved organic matter in secondary effluent during granular activated carbon treatment. JournalβofβZhejiangβUniversity-ScienceβA , 2008, 9(7): 994-1003
doi: 10.1631/jzus.A071508
13 Kweon J H, Hur H W, Seo G T, Jang T R, Park J H, Choi K Y, Kim H S. Evaluation of coagulation and PAC adsorption pretreatments on membrane filtration for a surface water in Korea: a pilot study. Desalination , 2009, 249(1): 212-216
doi: 10.1016/j.desal.2008.08.014
14 Wei L L, Zhao Q L, Xue S, Chang C C, Tang F, Liang G L, Jia T. Reduction of trihalomethane precursors of dissolved organic matter in the secondary effluent by advanced treatment processes. Journal of Hazardous Materials , 2009, 169(1-3): 1012-1021
doi: 10.1016/j.jhazmat.2009.04.045 pmid:19443112
15 Gur-Reznik S, Katz I, Dosoretz C G. Removal of dissolved organic matter by granular activated carbon adsorption as a pretreatment to reverse osmosis of membrane bioreactor effluents. Water Research , 2008, 42(6-7): 1595-1605
doi: 10.1016/j.watres.2007.10.004 pmid:17980400
16 Luciani X, Mounier S, Paraquetti H H M, Redon R, Lucas Y, Bois A, Lacerda L D, Raynaud M, Ripert M. Tracing of dissolved organic matter from the Sepetiba Bay (Brazil) by PARAFAC analysis of total luminescence matrices. Marine Environmental Research , 2008, 65(2): 148-157
doi: 10.1016/j.marenvres.2007.09.004 pmid:17976715
17 Yamashita Y, Tanoue E. Chemical characterization of protein-like fluorophores in DOM in relation to aromatic amino acids. Marine Chemistry , 2003, 82(3-4): 255-271
doi: 10.1016/S0304–4203(03)00073–2
18 Chen J, Gu B, Leboeuf E J, Pan H, Dai S. Spectroscopic characterization of the structural and functional properties of natural organic matter fractions. Chemosphere , 2002, 48(1): 59-68
doi: 10.1016/S0045–6535(02)00041–3 pmid:12137058
19 Chen J, LeBoeuf E J, Dai S, Gu B. Fluorescence spectroscopic studies of natural organic matter fractions. Chemosphere , 2003, 50(5): 639-647
doi: 10.1016/S0045–6535(02)00616–1 pmid:12685740
20 Kim H C, Yu M J. Characterization of natural organic matter in conventional water treatment processes for selection of treatment processes focused on DBPs control. Water Research , 2005, 39(19): 4779-4789
doi: 10.1016/j.watres.2005.09.021 pmid:16253305
21 Aiken G R, McKnight D M, Thorn K A, Thurman E M. Isolation of hydrophilic organic acids from water using nonionic macroporous resins. Organic Geochemistry , 1992, 18(4): 567-573
doi: 10.1016/0146–6380(92)90119–I
22 Chow A T, Guo F, Gao S, Breuer R S. Size and XAD fractionations of trihalomethane precursors from soils. Chemosphere , 2006, 62(10): 1636-1646
doi: 10.1016/j.chemosphere.2005.06.039 pmid:16095666
23 McKnight D M, Boyer E W, Westerhoff P K, Doran P T, Kulbe T, Andersen D T. Spectrofluorometric characterization of dissolved organic matter for indication of precursor organic materials and aromaticity. Limnology and Oceanography , 2001, 46(1): 38-48
doi: 10.4319/lo.2001.46.1.0038
24 Xiao X, Zhang Y J, Wang Z G, Jin D, Yin G F, Zhao N J, Liu W Q. Experimental studies on three-dimensional fluorescence spectral of mineral oil in ethanol. SpectroscopyβandβSpectralβAnalysis , 2010, 30(6): 1549-1554
25 Chen W, Westerhoff P, Leenheer J A, Booksh K. Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter. Environmental Science & Technology , 2003, 37(24): 5701-5710
doi: 10.1021/es034354c pmid:14717183
26 Panyapinyopol B, Marhaba T F, Kanokkantapong V, Pavasant P. Characterization of precursors to trihalomethanes formation in Bangkok source water. Journal of Hazardous Materials , 2005, 120(1-3): 229-236
doi: 10.1016/j.jhazmat.2005.01.009 pmid:15811685
27 Kanokkantapong V, Marhaba T F, Pavasant P, Panyapinyophol B. Characterization of haloacetic acid precursors in source water. Journal of Environmental Management , 2006, 80(3): 214-221
doi: 10.1016/j.jenvman.2005.09.006 pmid:16377072
28 Hur J, Jung N C, Shin J K. Spectroscopic distribution of dissolved organic matter in a dam reservoir impacted by turbid storm runoff. Environmental Monitoring and Assessment , 2007, 133(1-3): 53-67
doi: 10.1007/s10661–006–9559–0 pmid:17286180
29 Drewes J E, Quanrud D M, Amy G L, Westerhoff P K. Character of organic matter in soil–aquifer treatment systems. Journal of Environmental Engineering , 2006, 132(11): 1447-1458
doi: 10.1061/(ASCE)0733–9372(2006)132:11(1447)
30 Maie N, Scully N M, Pisani O, Jaffé R. Composition of a protein-like fluorophore of dissolved organic matter in coastal wetland and estuarine ecosystems. Water Research , 2007, 41(3): 563-570
doi: 10.1016/j.watres.2006.11.006 pmid:17187842
31 Sierra M M D, Giovanela M, Parlanti E, Soriano Sierra E J. Fluorescence fingerprint of fulvic and humic acids from varied origins as viewed by single-scan and excitation/emission matrix techniques. Chemosphere , 2005, 58(6): 715-733
doi: 10.1016/j.chemosphere.2004.09.038 pmid:15621185
32 Vo Dinh T. Multicomponent analysis by synchronous lumines cence spectrometry. Analytical Chemistry , 1978, 50(3): 396-401
doi: 10.1021/ac50025a010
33 Peuravuori J, Koivikko R, Pihlaja K. Characterization, differentiation and classification of aquatic humic matter separated with different sorbents: synchronous scanning fluorescence spectroscopy. Water Research , 2002, 36(18): 4552-4562
doi: 10.1016/S0043–1354(02)00172–0 pmid:12418658
34 Zhang T, Lu J F, Ma J, Qiang Z. Fluorescence spectroscopic characterization of DOM fractions isolated from a filtered river water after ozonation and catalytic ozonation. Chemosphere , 2008, 71(5): 911-921
doi: 10.1016/j.chemosphere.2007.11.030 pmid:18190948
35 Fabbricino M, Korshin G V. Probing the mechanisms of NOM chlorination using fluorescence: formation of disinfection by-products in Alento River water. Water Science and Technology: Water Supply , 2004, 4(4): 227-233
36 Kim H C, Yu M J, Han I. Multi-method study of the characteristic chemical nature of aquatic humic substances isolated from the Han River, Korea. Applied Geochemistry , 2006, 21(7): 1226-1239
doi: 10.1016/j.apgeochem.2006.03.011
Related articles from Frontiers Journals
[1] Xia Hou, Liping Huang, Peng Zhou, Hua Xue, Ning Li. Response of indigenous Cd-tolerant electrochemically active bacteria in MECs toward exotic Cr(VI) based on the sensing of fluorescence probes[J]. Front. Environ. Sci. Eng., 2018, 12(4): 7-.
[2] Yu Liu, Qiao Zhang, Yu Hong. Formation of disinfection byproducts from accumulated soluble products of oleaginous microalga after chlorination[J]. Front. Environ. Sci. Eng., 2017, 11(6): 1-.
[3] Yun Zhou, Siqing Xia, Binh T. Nguyen, Min Long, Jiao Zhang, Zhiqiang Zhang. Interactions between metal ions and the biopolymer in activated sludge: quantification and effects of system pH value[J]. Front. Environ. Sci. Eng., 2017, 11(1): 7-.
[4] Rui Lu, Wei Chen, Wen-Wei Li, Guo-Ping Sheng, Lian-Jun Wang, Han-Qing Yu. Probing the redox process of p-benzoquinone in dimethyl sulphoxide by using fluorescence spectroelectrochemistry[J]. Front. Environ. Sci. Eng., 2017, 11(1): 14-.
[5] Yuan ZHANG,Chunming HU,Tao YU. Photodegradation of chromophoric dissolved organic matters in the water of Lake Dianchi, China[J]. Front. Environ. Sci. Eng., 2015, 9(4): 575-582.
[6] Hongguang CHENG,Xiao PU,Yiting CHEN,Fanghua HAO,Liming DONG. Characterization of phosphorus species and modeling for its organic forms in eutrophic shallow lake sediments, North China[J]. Front. Environ. Sci. Eng., 2014, 8(6): 905-921.
[7] Yuan ZHANG,Yan ZHANG,Tao YU. Quantitative characterization of Cu binding potential of dissolved organic matter (DOM) in sediment from Taihu Lake using multiple techniques[J]. Front.Environ.Sci.Eng., 2014, 8(5): 666-674.
[8] Yan ZHANG,Yuan ZHANG,Tao YU. Characterization of interaction between different adsorbents and copper by simulation experiments using sediment-extracted organic matter from Taihu Lake, China[J]. Front.Environ.Sci.Eng., 2014, 8(4): 510-518.
[9] Gang GUO, Yayi WANG, Chong WANG, Hong WANG, Mianli PAN, Shaowei CHEN. Short-term effects of excessive anaerobic reaction time on anaerobic metabolism of denitrifying polyphosphate- accumulating organisms linked to phosphorus removal and N2O production[J]. Front Envir Sci Eng, 2013, 7(4): 616-624.
[10] 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.
[11] Shucai LI, Tingting LI, Gang LI, Fengmei LI, Shuhai GUO. Enhanced electrokinetic remediation of chromium-contaminated soil using approaching anodes[J]. Front Envir Sci Eng, 2012, 6(6): 869-874.
[12] Xiangliang PAN, Jing LIU, Wenjuan SONG, Daoyong ZHANG. Biosorption of Cu(II) to extracellular polymeric substances (EPS) from Synechoeystis sp.: a fluorescence quenching study[J]. Front Envir Sci Eng, 2012, 6(4): 493-497.
[13] Jing ZHANG, Shigong WANG, Can WANG, Hongying HU. Chemical identification and genotoxicity analysis of petrochemical industrial wastewater[J]. Front Envir Sci Eng, 2012, 6(3): 350-359.
[14] Fang FANG, Yan YANG, Jinsong GUO, Hong ZHOU, Chuan FU, Zhe LI. Three-dimensional fluorescence spectral characterization of soil dissolved organic matters in the fluctuating water-level zone of Kai County, Three Gorges Reservoir[J]. Front Envir Sci Eng Chin, 2011, 5(3): 426-434.
Full text