丝状真菌黑曲霉对放射性核素U(Ⅵ)的吸附、富集和转化
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摘要
本文采用批试验和X射线吸收精细结构谱学(XAFS)技术系统研究了黑曲霉菌丝体对放射性核素U(Ⅵ)的吸附、富集和转化.宏观研究表明,时间、菌丝体浓度、pH和温度显著影响菌丝体吸附U(Ⅵ),吸附动力学符合准二级动力学模型;吸附等温线符合Langmuir模型,在pH 6.0, T=298 K条件下,菌丝体吸附U(Ⅵ)的最大吸附量是83.73 mg/g,比其他生物吸附剂有较高的吸附U(Ⅵ)能力.黑曲霉富集U(Ⅵ)后,胞内外形态结构明显改变,并且胞内H_2O_2、丙二醛(MDA)和巯基化合物浓度显著增加.使用X射线吸收近边缘结构(XANES)分析证实黑曲霉胞内U(Ⅵ)减少,被还原为U(Ⅳ);扩展X射线吸收精细结构(EXAFS)数据表明, U(Ⅳ)产物是由单核U(Ⅳ)原子紧密包围的轻元素壳组成的形态,这种原子排列可能由U(Ⅳ)和C/N/O–或含P/S的配体(如碳酸根或磷酸根)之间的内球键产生.研究结果表明,丝状真菌黑曲霉有望应用于放射性核素U(Ⅵ)污染的修复治理.
The adsorption, bioconcentration and transformation of radionuclides U(Ⅵ) by Aspergillus niger(A. niger)were studied. Batch experiments showed that the adsorption of U(Ⅵ) by A. niger was influenced by time, adsorbent concentration, pH value and temperature. The adsorption reached equilibrium within 48 h, and the adsorption kinetics complied with the pseudo-second-order kinetics model. The Langmuir model was more consistent with the adsorption isotherm than the Freundlich model, and the maximum adsorption of U(Ⅵ) by mycelia was 83.73 mg/g at pH 6.0 and T=298 K, which was higher than other biosorbents. After bioconcentration of U(Ⅵ) by A. niger, the intracellular and extracellular morphological structures changed significantly, and the concentrations of intracellular H_2O_2,malonaldehyde(MDA) and thiol compounds in mycelia increased obviously. X-ray absorption near-edge structure(XANES) analysis confirmed that the intracellular U(Ⅵ) of A. niger was reduced to U(Ⅳ), and EXAFS data indicated that the U(Ⅳ) product was a phase composed of mononuclear U(Ⅳ) atoms closely surrounded by light element shells.The results showed that the filamentous fungus A. niger can be used as a potential biological material for radionuclide removal, which has important scientific significance and potential application value.
The adsorption, bioconcentration and transformation of radionuclides U(Ⅵ) by Aspergillus niger(A. niger)were studied. Batch experiments showed that the adsorption of U(Ⅵ) by A. niger was influenced by time, adsorbent concentration, pH value and temperature. The adsorption reached equilibrium within 48 h, and the adsorption kinetics complied with the pseudo-second-order kinetics model. The Langmuir model was more consistent with the adsorption isotherm than the Freundlich model, and the maximum adsorption of U(Ⅵ) by mycelia was 83.73 mg/g at pH 6.0 and T=298 K, which was higher than other biosorbents. After bioconcentration of U(Ⅵ) by A. niger, the intracellular and extracellular morphological structures changed significantly, and the concentrations of intracellular H_2O_2,malonaldehyde(MDA) and thiol compounds in mycelia increased obviously. X-ray absorption near-edge structure(XANES) analysis confirmed that the intracellular U(Ⅵ) of A. niger was reduced to U(Ⅳ), and EXAFS data indicated that the U(Ⅳ) product was a phase composed of mononuclear U(Ⅳ) atoms closely surrounded by light element shells.The results showed that the filamentous fungus A. niger can be used as a potential biological material for radionuclide removal, which has important scientific significance and potential application value.
引文
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2 Zheng T,Yang Z,Gui D,Liu Z,Wang X,Dai X,Liu S,Zhang L,Gao Y,Chen L,Sheng D,Wang Y,Diwu J,Wang J,Zhou R,Chai Z,AlbrechtSchmitt TE,Wang S.Nat Commun,2017,8:15369
3 Cai Y,Wu C,Liu Z,Zhang L,Chen L,Wang J,Wang X,Yang S,Wang S.Environ Sci-Nano,2017,4:1876-1886
4 Geckeis H,Lützenkirchen J,Polly R,Rabung T,Schmidt M.Chem Rev,2013,113:1016-1062
5 Pang H,Wang X,Yao W,Yu S,Wang X.Sci Sin Chim,2018,48:58-73(in Chinese)[庞宏伟,王祥学,姚文,于淑君,王祥科.中国科学:化学,2018,48:58-73]
6 Sheng D,Zhu L,Xu C,Xiao C,Wang Y,Wang Y,Chen L,Diwu J,Chen J,Chai Z,Albrecht-Schmitt TE,Wang S.Environ Sci Technol,2017,51:3471-3479
7 Xu L,Zheng T,Yang S,Zhang L,Wang J,Liu W,Chen L,Diwu J,Chai Z,Wang S.Environ Sci Technol,2016,50:3852-3859
8 Liang Y,Gu P,Yao W,Yu S,Wang J,Wang X.Prog Chem,2017,29:1062-1071(in Chinese)[梁宇,顾鹏程,姚文,于淑君,王建,王祥科.化学进展,2017,29:1062-1071]
9 Sun Y,Lu S,Wang X,Xu C,Li J,Chen C,Chen J,Hayat T,Alsaedi A,Alharbi NS,Wang X.Environ Sci Technol,2017,51:12274-12282
10 Tkavc R,Matrosova VY,Grichenko OE,Gostin?ar C,Volpe RP,Klimenkova P,Malfatti SA.Front Microbial,2017,8:1-21
11 Vázquez-Campos X,Kinsela AS,Collins RN,Neilan BA,Aoyagi N,Waite TD.Environ Sci Technol,2015,49:8487-8496
12 Gadd GM,Fomina M.Geomicrobiol J,2011,28:471-482
13 Lujanien?G,Levinskait?L,Ka?ergius A,Gavutis M.J Radioanal Nucl Chem,2017,311:1393-1399
14 Vinichuk M,M?rtensson A,Ericsson T,Rosén K.J Environ Radioact,2013,115:151-156
15 Zhao C,Liu J,Tu H,Li F,Li X,Yang J,Liao J,Yang Y,Liu N,Sun Q.Environ Sci Pollut Res,2016,23:24846-24856
16 Ding C,Feng S,Li X,Liao J,Yang Y,An Z,Wu Q,Zhang D,Yang J,Tang J,Zhang J,Liu N.Radiochim Acta,2014,102:175-184
17 Song W,Liang J,Wen T,Wang X,Hu J,Hayat T,Alsaedi A,Wang X.Chem Eng J,2016,304:186-193
18 Jiang GCT,Hughes S,Stürzenbaum SR,Evje L,Syversen T,Aschner M.Toxicol Sci,2009,111:345-354
19 Xu P,Liu L,Zeng G,Huang D,Lai C,Zhao M,Huang C,Li N,Wei Z,Wu H,Zhang C,Lai M,He Y.Appl Microbiol Biotechnol,2014,98:6409-6418
20 Xu H,Song P,Gu W,Yang Z.Ecotoxicol Environ Saf,2011,74:1685-1692
21 Schneider J,Bundschuh J,Rangel WM,Guilherme LRG.Environ Pollut,2017,224:125-135
22 Günther A,Raff J,Merroun ML,Ro?berg A,Kothe E,Bernhard GI.Biometals,2014,27:775-785
23 Yu Q,Ohnuki T,Tanaka K,Kozai N,Yamasaki S,Sakamoto F,Tani Y.Geochim Cosmochim Acta,2016,174:1-12
24 Song W,Wang X,Chen Z,Sheng G,Hayat T,Wang X,Sun Y.Environ Pollut,2018,237:228-236
25 Mendil D,Do?an Ulu?zlü?,Hasdemir E,Tüzen M,Sari H,Sui?mez M.Food Chem,2005,90:175-179
26 Guimar?es-Soares L,Pascoal C,Cássio F.Ecotoxicol Environ Saf,2007,66:36-43
27 van Veelen A,Bargar JR,Law GTW,Brown Jr GE,Wogelius RA.Environ Sci Technol,2016,50:3435-3443
28 Sun Y,Li J,Wang X.Geochim Cosmochim Acta,2014,140:621-643
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32 Yang S,Zong P,Hu J,Sheng G,Wang Q,Wang X.Chem Eng J,2012,214:376-385
33 Ding DX,Liu XT,Hu N,Li GY,Wang YD.J Radioanal Nucl Chem,2012,293:735-741
34 Song M,Wang Q,Meng Y.J Radioanal Nucl Chem,2012,293:899-906
35 Shao D,Jiang Z,Wang X,Li J,Meng Y.J Phys Chem B,2009,113:860-864
36 Aytas S,Turkozu DA,Gok C.Desalination,2011,280:354-362
37 Han R,Zou W,Wang Y,Zhu L.J Environ Radioact,2007,93:127-143
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40 O’Loughlin EJ,Kelly SD,Kemner KM.Environ Sci Technol,2010,44:1656-1661
41 Troyer LD,Tang Y,Borch T.Environ Sci Technol,2014,48:14326-14334
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43 Smith H,Doyle S,Murphy R.Food Chem,2015,185:389-397
44 Bernier-Latmani R,Veeramani H,Vecchia ED,Junier P,Lezama-Pacheco JS,Suvorova EI,Sharp JO,Wigginton NS,Bargar JR.Environ Sci Technol,2010,44:9456-9462
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