Effect of electron transfer on the structure of dissolved organic matter during initial landfill stage
YANG Chao1,2,3, HE Xiao-song1,2, XI Bei-dou1,2,3, ZHANG Hui1,2, HUANG Cai-hong1,2, GAO Ru-tai1,2, TAN Wen-bing1,2, CUI Dong-yu1,2
1. State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China;
2. State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Science, Beijing 100012, China;
3. School of Environmental and Municipal Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China
In order to investigate the structural change of dissolved organic matter after electron transfer, dissolved organic matter (DOM) were extracted fromlandfilled wastes at different depthsduring initial landfill stage, and shewanella Shewanella MR-1 and citrate iron (FeCit) were used as electron donor and electronacceptor, respectively. Furtherover, fluorescence excitation-emission matrix (EEM) spectra combined with parallel factor (PARAFAC) analysis was used to analyze the structure change of DOM. The results indicated that four fluorescent components, i.e., two humic-like components (C2 and C4) and two protein-like components (C1 and C3), were identified by the PARAFAC analysis, and protein-like components was the major component. The nitrogen-containing heterocyclic structure was desassembled when protein-like components got electrons, and theirhydrophobicity and fluorescence intensities were increased during the process. Fluorescence intensities of humic-like components were increased as well when they obtained electrons, though their increased range became decrease during the landfill processs. The carbonyl group on humic-like components were turn into alcohol group when it obatained electrons. Fluorescence quenching phenomenon was observeredwhen DOM loss electrons. Protein-like components wereable to offerelectrons, and theirstructure changed after they loss electrons. Humic-like substances can offer electrons as well, and their fluorescence intensities decreased as well when they loss electrons. However, the decreased range was related to the content of carboxyl and phenolic groups on humic-like subtaneces. Humic-like components could bereoxided, However, protein-like components could not be reduced after they was oxided. The electron shuttle capacityof DOM were ascribed to humic-like components, which were persistentlyincreasedduring the landfill process.
杨超, 何小松, 席北斗, 张慧, 黄彩红, 高如泰, 檀文炳, 崔东宇. 填埋初期水溶性有机物结构受电子转移的影响[J]. 中国环境科学, 2017, 37(1): 229-237.
YANG Chao, HE Xiao-song, XI Bei-dou, ZHANG Hui, HUANG Cai-hong, GAO Ru-tai, TAN Wen-bing, CUI Dong-yu. Effect of electron transfer on the structure of dissolved organic matter during initial landfill stage. CHINA ENVIRONMENTAL SCIENCECE, 2017, 37(1): 229-237.
He X, XI B, Wei Z, Guo X, et al. Spectroscopic characterization of water-extractable organic matter during composting of municipal solid waste[J]. Chemosphere, 2011,2(4):541-548.
[2]
Bi R, Lu Q, Yu W M, Zhou S G. Electron transfer capacity of soil dissolved organic matter and its potential impact on soil respiration[J]. Journal of Soils and Sediments, 2013,13(9):1553-1560.
[3]
He X S, Xi B D, Cui D Y, et al. Influence of chemical and structural evolution of dissolved organic matter on electron transfer capacity during composting[J]. Journal of Hazardous Materials, 2014,268(15):256-263.
[4]
Wagner S, JaFFE R, Cawley K, et al. Associations between the molecular and optical properties of dissolved organic matter in the Florida Everglades, a model coastal wetland system[J]. Fronts in Chemistry, 2015,26(2):1-14.
[5]
Lavonen E E, Kothawala D N, Tranvik L J, et al. Tracking changes in the optical properties and molecular composition of dissolved organic matter during drinking water production[J]. Water Research, 2015,85(15):286-294.
[6]
Opsahl S, Benner R. Distribution and cycling of terrigenous dissolve dorganic matter in the ocean[J]. Nature, 1997,386(16):480-482.
[7]
Spencer R G M, Mann P J, Dittmar T, et al. Detecting the signature of permafrost thaw in Arctic rivers[J]. Geophysical Research Letters, 2015,42(8):2830-2835.
[8]
Plaza C, Xing B, Fernández J M, et al. Binding of polycyclic aromatic hydrocarbons by humic acids formed during composting[J]. Environmental Pollution, 2009,157(1):257-263.
[9]
Xi B D, He X S, Wei Z M, et al. The composition and mercury complexation characteristics of dissolved organic matter in landfill leachates with different ages[J].Ecotoxicology and Environmental safety, 2012,86(1):227-232.
[10]
Yuan T, Yuan Y, Zhou S G, et al. A rapid and simple electrochemical method for evaluating the electron transfer capacities of dissolved organic matter[J]. Journal of Soils and Sediments, 2011,11(3):467-473.
[11]
Zhu Z, Tao L, Li F. Effects of dissolved organic matter on adsorbed Fe(Ⅱ) reactivity for the reduction of 2-nitrophenol in TiO2 suspensions[J]. Chemosphere, 2013,93(1):29-34.
Huo S L, Xi B D, Yu H C, et al. Characteristics of dissolved organic matter (DOM) in leachate with different landfill ages[J]. Journal of Environmental Sciences, 2008,20(4):492-498.
[14]
Klapper L, McKnight D M, Fulton J R, et al.Fulvic acid oxidation state detection using fluorescence spectroscopy[J]. Environment Science and Technology, 2002,36(14):3170-3175.
[15]
Ma J H, Vecchio R A, Golanoski K S, et al. Optical properties of humic substances and CDOM:effects of borohydride reduction[J]. Environment Science and Technology, 2010,44(14):6395- 5402.
[16]
Cory R M, Mcknight D M. Fluorescence spectroscopy eeveals ubiquitous presence of oxidized and reduced quinones in dissolved organic matter[J]. Environment Science and Technology, 2005,39(21):8142-8149.
[17]
Boyle S, Guerriero S, Thiallet A, et al. Optical properties of humic substances and CDOM:relation to structure[J]. Environmental Science & Technology, 2009,43(7):2262-2268.
[18]
Phillips S M, Smith G D. Further evidence for charge transfer complexes in brown carbon aerosols from excitation-emission matrix fluorescence spectroscopy[J]. The Journal of Physical Chemistry A, 2012,119(19):4545-4551.
[19]
Guo R R, Ma J H. Reduction-induced molecular signature of humic substances:structural evidence for optical changes[J]. The Royal Society of Chemistry, 2014,4(49):25880-25885.
[20]
Helms J R, Stubbins A, Ritchie J D, et al. Absorption spectral slopes and slope ratios as indicators of molecular weight, source, and photobleaching of chromophoric dissolved organic matter[J]. Limnology and Oceanography, 2008,53(3):955-969.
[21]
Chen W, Westerhoff P, Leenheer J A, et al. Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter[J]. Environmental Science & Technology, 2003,37(24):5701-5710.
Baker A, Curry M. Fluorescence of leachates from three ontrasting landfills[J]. Water Research, 2004,38(10):2605-2613.
[26]
Yamashita Y, Jaffe R. Characterizing the interactions between trace metals and dissolved organic matter using excitationemission matrix and parallel factor analysis[J]. Environmental Science & Technology, 2008,42(19):7374-7379.
[27]
Shao Z H, He P J, Zhang D Q, et al. Characterization of water- extractable organic matter during the biostabilization of municipal solid waste[J]. Journal of Hazardous Materials, 2009,164(2/3):1191-1197.
[28]
Coble P G. Characterization of marine and terrestrial DOM in seawater using excitation-emission matrix spectroscopy[J]. Marine Chemistry, 1996,51(4):325-346.
[29]
Haas J R, Dichristina T J. Effects of Fe(Ⅲ) Chemical Speciation on Dissimilatory Fe(Ⅲ) Reduction by Shewanella putrefaciens[J]. Environment Science and Technology, 2002,36(3):373-380.
[30]
Vecchio R D, Blough N V. On the origin of the optical properties of humic substances.[J]. Environmental Science & Technology, 2004,38(14):3885-3891.
Macalady D L, Walton-Doy K. New light on a dark subject:On the use of fluorescence data to deduce redox states of natural organic matter (NOM)[J]. Aquatic Sciences, 2009,71(2):135- 142.
Klapper L, McKnight D M, Fulton J R, et al. Fulvic acid oxidation state detection using fluorescence spectroscopy[J]. Environmental Science & Technology, 2002,36(14):3170-3175.
[35]
Aeschbacher M, Sander M, Schwarzenbach R P. Novel electrochemical approach to assess the redox properties of humic substances[J]. Environmental Science & Technology, 2010,44(1):87-93.
[36]
Stevenson F J. Humus chemistry:genesis, composition, reactions[M]. NewYork:John Wiley and Sons, 1982.
[37]
He X S, Xi B D, Wei Z M, et al. Physicochemical and spectroscopic characteristics of dissolved organic matter extracted from municipal solid waste (MSW) and their influence on the landfill biological stability[J]. Bioresource Technology, 2011, 102(3):2322-2327.