生物炭改性高庙子膨润土对铕(Ⅲ)的吸附特性
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摘要
针对作为我国核废料处置库缓冲/回填材料——高庙子(GMZ)膨润土——在长期运营条件下的缓冲性能衰减问题,利用梧桐叶为碳源制备生物炭改性GMZ膨润土,通过微观表征和批次吸附试验,研究了其结构和对Eu(Ⅲ)的吸附性能,进一步探讨了复合材料的作用机理.结果表明,生物炭改性GMZ膨润土中的官能团出现次甲基(—CH),说明有机官能团嫁接成功,层间距进一步增大,蒙脱石表面的细小颗粒在改性后变大.在吸附性能方面,随着固液比和接触时间的增加,吸附率提高;随着pH值、离子强度的增加,吸附率降低;生物炭改性GMZ膨润土对Eu(Ⅲ)的吸附等温线符合Langmuir模型和准二级动力学模型,最大理论吸附量为32.36 mg·g~(-1).
Aimed at the buffer performance degradation problem of GMZ bentonite, which is the cushioning backfill material of China's nuclear waste repository in long-term operation, the biochar modified GMZ bentonite was prepared by using the leaves of Davidia involucrata as carbon source. The microstructure and adsorption performance of Eu(Ⅲ) were studied by microscopic characterization and batch adsorption experiments. The mechanism of the composite was further discussed. The results showed that methine(—CH) appeared in the functional group of biochar modified GMZ bentonite, indicating the fact that the organic light energy group grafting was successful; the interlayer spacing was further increased, and the fine particles on the surface of montmorillonite became larger after modification. In terms of adsorption performance, with the increase of solid-liquid ratio and contact time, the adsorption rate increases while with the increase of pH value and ionic strength, the adsorption rate decreases. The adsorption isotherm of bio-carbon modified GMZ bentonite to Eu(Ⅲ). The Langmuir model and the quasi-secondary kinetic model have a maximum theoretical adsorption capacity of 32.36 mg·g~(-1).
Aimed at the buffer performance degradation problem of GMZ bentonite, which is the cushioning backfill material of China's nuclear waste repository in long-term operation, the biochar modified GMZ bentonite was prepared by using the leaves of Davidia involucrata as carbon source. The microstructure and adsorption performance of Eu(Ⅲ) were studied by microscopic characterization and batch adsorption experiments. The mechanism of the composite was further discussed. The results showed that methine(—CH) appeared in the functional group of biochar modified GMZ bentonite, indicating the fact that the organic light energy group grafting was successful; the interlayer spacing was further increased, and the fine particles on the surface of montmorillonite became larger after modification. In terms of adsorption performance, with the increase of solid-liquid ratio and contact time, the adsorption rate increases while with the increase of pH value and ionic strength, the adsorption rate decreases. The adsorption isotherm of bio-carbon modified GMZ bentonite to Eu(Ⅲ). The Langmuir model and the quasi-secondary kinetic model have a maximum theoretical adsorption capacity of 32.36 mg·g~(-1).
引文
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[24] ABROMAITIS V,RACYS V,VAN DER MAREL P,et al.Biodegradation of persistent organics can overcome adsorption-desorption hysteresis in biological activated carbon systems[J].Chemosphere,2016,149:183.
[25] VIEIRA M G A,NETO A F A,GIMENES M L,et al.Sorption kinetics and equilibrium for the removal of nickel ions from aqueous phase on calcined Bofe bentonite clay[J].Journal of Hazardous Materials,2010,177(1/2/3):362.
[2] CHEN X,WU L,LIU F,et al.Performance and mechanisms of thermally treated bentonite for enhanced phosphate removal from wastewater[J].Environmental Science and Pollution Research,2018,25(16):15980.
[3] MORADI N,SALEM S,SALEM A.Optimizing adsorption of blue pigment from wastewater by nano-porous modified Na-bentonite using spectrophotometry based on response surface method[J].Spectrochim Acta A Mol Biomol Spectrosc,2018,193:54.
[4] DEMDOUM A,GUEDDOUDA M K,GOUAL I.Effect of water and leachate on hydraulic behavior of compacted bentonite,calcareous sand and tuff mixtures for use as landfill liners[J].Geotechnical & Geological Engineering,2017,35(9):1.
[5] VILLAR M V,MARTíN P L,BáRCENA I,et al.Long-term experimental evidences of saturation of compacted bentonite under repository conditions[J].Engineering Geology,2012,149/150(4):57.
[6] 王所伟,李家星,陈磊,等.Th((Ⅵ)在高庙子膨润土上的吸附行为 [J].核化学与放射化学,2010,32(2):106.WANG Suowei,LI Jiaxing,CHEN Lei,et al.Adsorption behavior of Th(Ⅵ) on Gaomiaozi bentonite[J].Nuclear Chemistry and Radiochemistry,2010,32(2):106.
[7] 姚军,苏锡光,龙会遵,等 .237Np(Ⅴ) 在膨润土上的吸附行为研究 [J].核化学与放射化学,2003,23(2):102.YAO Jun,SU Xiguang,LONG Huizun,et al.Study on adsorption behavior of 237Np(Ⅴ) on bentonite[J].Nuclear Chemistry and Radiochemistry,2003,23(2):102.
[8] 靳强.U(Ⅵ)、Th(Ⅳ)、Eu(Ⅲ)/Am(Ⅲ)在北山花岗岩和高庙子膨润土上的吸附作用:温度和腐殖质的效应[D].兰州:兰州大学,2017.JIN Qiang.Adsorption of U(Ⅵ),Th(Ⅳ),Eu(Ⅲ)/Am(Ⅲ) on Beishan granite and Gaomiaozi bentonite:effects of temperature and humus [D].Lanzhou:Lanzhou University,2017.
[9] SADEGHALVAD B,AZADMEHR A R,MOTEVALIAN H.Statistical design and kinetic and thermodynamic studies of Ni(Ⅱ) adsorption on bentonite[J].Journal of Central South University,2017,24(7):1529.
[10] WANG J Q,CHEN Z,SHAO D D,et al.Adsorption of U(Ⅵ) on bentonite in simulation environmental conditions[J].Journal of Molecular Liquids,2017,242:678.
[11] 李平.Eu(Ⅲ)、Th(Ⅳ)、U(Ⅵ)在铁氧化物及Np(V)在钠基膨润土上的吸附行为研究[D].兰州:兰州大学,2015.LI Ping.Adsorption behavior of Eu(Ⅲ),Th(Ⅳ) and U(Ⅵ) on iron oxide and Np(Ⅴ) on sodium bentonite[D].Lanzhou:Lanzhou University,2015.
[12] WANG X X,SUN Y B,ALSAEDI A,et al.Interaction mechanism of Eu(Ⅲ) with MX-80 bentonite studied by batch,TRLFS and kinetic desorption techniques[J].Chemical Engineering Journal,2015,264:570.
[13] LI D M,ZHANG B,XUAN F Q.The sorption of Eu(Ⅲ) from aqueous solutions by magnetic graphene oxides:a combined experimental and modeling studies[J].Journal of Molecular Liquids,2015(211):570.
[14] 成龙,梁吉艳,姜伟,等.改性膨润土吸附处理重金属离子的研究进展[J].安徽农业科学,2017,45(10):53.CHENG Long,LIANG Jiyan,JIANG Wei,et al.Advances in a dsorption of heavy metal Ions by modified bentonite[J].Anhui Agricultural Sciences,2017,45(10):53.
[15] LIU J,NERETNIEKS I.Physical and chemical stability of the bentonite buffer[R].Stockholm:Swedish Nuclear Fuel and Waste Management Company,2007.
[16] GHADR S,ASSADI-LANGROUDI A.Structure-based hydro-mechanical properties of sand-bentonite composites[J].Engineering Geology,2018,235:53.
[17] BALLARINI E,GRAUPNER B,BAUER S.Thermal-hydraulic-mechanical behavior of bentonite and sand-bentonite materials as seal for a nuclear waste repository:numerical simulation of column experiments[J].Applied Clay Science,2017,135:289.
[18] NGUEMTCHOUIN M G M,NGASSOUM,M B,KAMGA R,et al.Characterization of inorganic and organic clay modified materials:an approach for adsorption of an insecticidal terpenic compound[J].Applied Clay Science,2015,104:110.
[19] LIANG H N,LONG Z,YANG S H,et al.Organic modification of bentonite and its effect on rheological properties of paper coating[J].Applied Clay Science,2015,104:106.
[20] 程君华.改性膨润土负载Au催化剂的制备及其催化氧化CO性能研究[D].南昌:南昌大学,2016.CHENG Junhua.Investigation on the preparation of modified bentonite supported Au catalysts and their catalytic performance for CO oxidation[D].Nanchang:Nanchang University,2016.
[21] FEHERVARI W P,GATES T W,TURNEY A F,et al.Cyclic organic carbonate modification of sodium bentonite for enhanced containment of hyper saline leachates[J].Applied Clay Science,2016,134:2.
[22] MOHAMMED M I,BAYTAK S.Synthesis of bentonite-carbon nanotube nanocomposite and its adsorption of rhodamine dye from water[J].Arabian Journal for Science and Engineering,2016,41(12):4775.
[23] HAGHSERESHT F,WANG S,DO D D.A novel lanthanum-modified bentonite,phoslock,for phosphate removal from wastewaters[J].Applied Clay Science,2009,46(4):369.
[24] ABROMAITIS V,RACYS V,VAN DER MAREL P,et al.Biodegradation of persistent organics can overcome adsorption-desorption hysteresis in biological activated carbon systems[J].Chemosphere,2016,149:183.
[25] VIEIRA M G A,NETO A F A,GIMENES M L,et al.Sorption kinetics and equilibrium for the removal of nickel ions from aqueous phase on calcined Bofe bentonite clay[J].Journal of Hazardous Materials,2010,177(1/2/3):362.