新型高效除砷分子筛的制备及吸附特性研究

Q2 Environmental Science 环境科学研究 Pub Date : 2020-09-01 DOI:10.13198/J.ISSN.1001-6929.2020.03.19
许江城, 康得军, 赵颖, 王宏亮, 龚天成, 陈其晓, 瞿聪, 杨天学
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引用次数: 1

摘要

为了提高4A分子筛对水溶液中砷的吸附性能,以质谱为载体,制备了载铁分子筛(FMS)和铁锰分子筛(FMMS)作为浸渍法除砷的吸附剂。采用SEM、FT-IR和BET对质谱和FMMS进行了表征,并进行了批量实验,考察了FMS和FMMS对五价砷(As^5+)和三价砷(As^3+)的吸附和去除效果。对FMS吸附过程进行了吸附动力学、等温吸附实验和吸附热力学研究。结果表明,FMS的比表面积显著增加,材料的表面结构得到改善。FMS的比表面积和孔体积分别从27.38 m^2 g和0.068 cm^3 g增加到281.25 m^2 g和0.16 cm^3 g。同时,平均孔径由9.93 nm减小到2.21 nm。这可能导致致密的粗颗粒成为具有松散多孔微观结构的吸附剂。FT-IR分析表明,在铁盐浸渍过程中形成的氧化铁主要以分子筛结构与O-H、Al-O和Si-O结合。4 mg L As^5+的批量实验结果表明,改性后的材料去除率提高了70%左右。吸附过程符合准二级吸附动力学,相关系数(r2)为0.99,说明化学吸附在吸附过程中起重要作用。Freundlich等温吸附模型与吸附数据拟合较好,相关系数(r2)为0.98,计算出最大吸附量为9.9 mg g.此外,热力学计算parametersΔG、ΔH andΔS发现温度升高有利于吸附,反应过程中物料表面固液之间的无序程度增大。与FMS相比,FMMS可以有效地提高As^3+的去除性能。当初始共存浓度为ρ(As^3+As^5+)=2.0、4.0、6.0 mg L时,FMMS的去除率分别提高了26.34%、28.06%和28.09%。研究表明,采用铁盐浸渍法对MS进行改性,可以有效提高MS对As^5+和As^3+的吸附能力,可以充分发挥该材料的实际应用价值。
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Preparation and Adsorption Characteristics of Novel Molecular Sieve for High Efficiency Arsenic Removal
In order to enhance the adsorption performance of 4A molecular sieve for arsenic in aqueous solution,using MS as a carrier,iron-loaded molecular sieves(FMS)and iron-manganese molecular sieves(FMMS)were prepared as adsorbents for arsenic removal by impregnation method.The MS and FMS were characterized by SEM,FT-IR and BET,and carried out batch experiments to investigate the adsorption and removal effects of FMS and FMMS for pentavalent arsenic(As^5+)and trivalent arsenic(As^3+).The adsorption kinetics,isothermal adsorption test and adsorption thermodynamics of the FMS adsorption process were performed.The results show that the specific surface area of FMS is significantly increased and the surface structure of the material is improved.The specific surface area and pore volume of the FMS increased from^27.38 m^2 g and 0.068 cm^3 g to 281.25 m^2 g and 0.16 cm^3 g,respectively.Meanwhile,the average pore size decreased from 9.93 nm to 2.21 nm.This could cause the dense coarse particles to become an adsorbent with loose porous microstructure.FT-IR analysis shows that iron oxide formed in the iron salt impregnation process is mainly combined with O-H,Al-O and Si-O in the molecular sieve structure.The results of batch experiments with 4 mg L As^5+indicate that the removal rate increases by about 70%after the material modification.Moreover,the adsorption process is in accordance with the quasi second-order adsorption kinetics,and the correlation coefficient(R 2)is 0.99,indicating that the chemical adsorption plays an important role in the adsorption process.The Freundlich isotherm adsorption model fits the adsorption data well with a correlation coefficient(R 2)is 0.98,and the maximum adsorption capacity is calculated to be 9.9 mg g.Furthermore,the calculation of thermodynamic parametersΔG,ΔH andΔS find that temperature increase is favorable for adsorption,and the disorder degree between solid and liquid on the surface of the material increases during the reaction.Compared with FMS,FMMS can effectively improve the removal performance of As^3+.The initial concentrationof coexistence conditions wereρ(As^3+As^5+)=2.0,4.0,6.0 mg L,the removal rate of FMMS is increased by about 26.34%,28.06%and 28.09%,respectively.The research shows that the use of iron salt impregnation method to modify MS can effectively increase the adsorption capacity of As^5+and As^3+,and can give full play to the practical application value of the material.
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环境科学研究
环境科学研究 Environmental Science-Environmental Science (miscellaneous)
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6496
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