磷酸盐共存对MOF-Fe吸附亚硒酸盐的影响
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摘要
通过系列吸附实验,研究了磷酸盐(Pi)共存对MOF-Fe吸附亚硒酸盐(Se(Ⅳ))的影响.结果表明,不加Pi的吸附体系(Pi/Se=0)中,Langmuir和Freundlich模型对MOF-Fe等温吸附Se(Ⅳ)的数据的拟合度都较高;体系中加入与Se(Ⅳ)等物质的量浓度的Pi(Pi/Se=1)以后,等温吸附过程只适合用Freundlich模型拟合.与Pi/Se=0体系相比,Pi/Se=1体系中MOF-Fe对Se(Ⅳ)的最大吸附容量降低了68%,而吸附亲和力和吸附异质性却明显增强.Pi/Se=0和1的两种体系中,MOF-Fe对Se(Ⅳ)的吸附平衡时间分别为160 min和40 min,二级动力学方程可很好地描述两种体系的动力学吸附过程,液膜扩散和颗粒内扩散是吸附反应的主要速率控制因子.两种体系中,MOF-Fe对Se(Ⅳ)的平衡吸附量均随着温度的升高而降低,吸附均属于自发放热且有序度降低的过程.与Pi/Se=0体系相比,Pi/Se=1体系中MOF-Fe对Se(Ⅳ)的平衡吸附量受温度影响更为明显,这说明升高温度增强了Pi对Se(Ⅳ)吸附在MOF-Fe上的竞争强度;Pi/Se=1体系中MOF-Fe对Se(Ⅳ)的吸附自由能ΔG~θ略微增大,而焓变ΔH~θ和熵变ΔS~θ均明显减小,这说明Pi共存导致MOF-Fe对Se(Ⅳ)的化学吸附贡献增强.吸附体系pH从4.0升高至8.0时,Pi/Se=0和1体系中MOF-Fe对Se(Ⅳ)的平衡吸附量分别降低了7%和37%.当增大体系中Pi的浓度时,MOF-Fe对Se(Ⅳ)的平衡吸附量呈指数模型降低并稳定于最大吸附量的30%,这表明MOF-Fe对Se(Ⅳ)的吸附中约70%的比例可归属为可逆吸附.可见,Pi/Se=1体系中MOF-Fe对Se(Ⅳ)的吸附可分为可逆和不可逆吸附,其中,可逆吸附受Pi的竞争作用影响而明显降低,不可逆吸附则不受共存Pi的影响.
The influence of phosphate(Pi) on selenite(Se(Ⅳ)) adsorption by MOF-Fe was investigated through the batch adsorption experiments that were conducted under different conditions. Results showed that in the system without Pi(Pi/Se=0) the isothermal adsorption data for Se(Ⅳ) by MOF-Fe could be well fitted by both Langmuir and Freundlich models(R~2=0.9855～0.9863). As for the system with a molar ratio of Pi/Se(Ⅳ)=1(Pi/Se=1), Freundlich model fitted the adsorption data better than Langmuir model, and the determination coefficients(R~2) of the two models were 0.9746 and 0.9374, respectively. Compared with the Pi/Se=0 system, the maximum adsorption capacity of Se(IV) by MOF-Fe in the Pi/Se=1 system decreased by 68%, while the adsorption affinity and adsorption heterogeneity enhanced significantly. In the two systems of Pi/Se=0 and 1, the equilibrium times of Se(IV) adsorption by MOF-Fe were 160 min and 40 min, respectively. The pseudo-second-order model was very suitable to describe the dynamic process of Se(IV) adsorption by MOF-Fe in the two systems, and film diffusion and intraparticle diffusion were the main rate control factors of the adsorption reactions. In the two systems, the amount of Se(IV) adsorbed on MOF-Fe decreased with increasing the temperature, and the adsorption process was spontaneous and the disorder after adsorption increased. Compared with the Pi/Se=0 system, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=1 system was more sensitive to the temperature, indicating that the competitive adsorption of Se(IV) by Pi increased with increasing the temperature. In the Pi/Se=1 system, the adsorption free energy of Se(IV) by MOF-Fe increased slightly, while the enthalpy and entropy reduced greatly, indicating that the coexistence of Pi increased the chemical adsorption of Se(IV) by MOF-Fe. Increasing the pH from 4.0 to 8.0, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=0 and 1 systems decreased by 7% and 37%, respectively. When the initial concentration of Pi was increased, the adsorption amount of Se(IV) by MOF-Fe was exponentially reduced, and then stabilized at about 30% of the maximum adsorption amount. This showed that about 70% of the maximum adsorption amount of could be attributed to the reversible for the Se(IV) adsorption by MOF-Fe. Therefore, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=1 system might include reversible and irreversible reactions, and the reversible reaction was significantly reduced due to the competitive effect of Pi, while the irreversible adsorption was hardly affected by the coexistence of Pi.
The influence of phosphate(Pi) on selenite(Se(Ⅳ)) adsorption by MOF-Fe was investigated through the batch adsorption experiments that were conducted under different conditions. Results showed that in the system without Pi(Pi/Se=0) the isothermal adsorption data for Se(Ⅳ) by MOF-Fe could be well fitted by both Langmuir and Freundlich models(R~2=0.9855～0.9863). As for the system with a molar ratio of Pi/Se(Ⅳ)=1(Pi/Se=1), Freundlich model fitted the adsorption data better than Langmuir model, and the determination coefficients(R~2) of the two models were 0.9746 and 0.9374, respectively. Compared with the Pi/Se=0 system, the maximum adsorption capacity of Se(IV) by MOF-Fe in the Pi/Se=1 system decreased by 68%, while the adsorption affinity and adsorption heterogeneity enhanced significantly. In the two systems of Pi/Se=0 and 1, the equilibrium times of Se(IV) adsorption by MOF-Fe were 160 min and 40 min, respectively. The pseudo-second-order model was very suitable to describe the dynamic process of Se(IV) adsorption by MOF-Fe in the two systems, and film diffusion and intraparticle diffusion were the main rate control factors of the adsorption reactions. In the two systems, the amount of Se(IV) adsorbed on MOF-Fe decreased with increasing the temperature, and the adsorption process was spontaneous and the disorder after adsorption increased. Compared with the Pi/Se=0 system, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=1 system was more sensitive to the temperature, indicating that the competitive adsorption of Se(IV) by Pi increased with increasing the temperature. In the Pi/Se=1 system, the adsorption free energy of Se(IV) by MOF-Fe increased slightly, while the enthalpy and entropy reduced greatly, indicating that the coexistence of Pi increased the chemical adsorption of Se(IV) by MOF-Fe. Increasing the pH from 4.0 to 8.0, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=0 and 1 systems decreased by 7% and 37%, respectively. When the initial concentration of Pi was increased, the adsorption amount of Se(IV) by MOF-Fe was exponentially reduced, and then stabilized at about 30% of the maximum adsorption amount. This showed that about 70% of the maximum adsorption amount of could be attributed to the reversible for the Se(IV) adsorption by MOF-Fe. Therefore, the adsorption of Se(IV) by MOF-Fe in the Pi/Se=1 system might include reversible and irreversible reactions, and the reversible reaction was significantly reduced due to the competitive effect of Pi, while the irreversible adsorption was hardly affected by the coexistence of Pi.
引文
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Khare N,Martin J D,Hesterberg D.2007.Phosphate bonding configuration on ferrihydrite based on molecular orbital calculations and XANES fingerprinting[J].Geochimica et Cosmochimica Acta,71(18):4405-4415
Krishna B S,Murty D S R,Jai Prakash B S.2000.Thermodynamics of chromium(VI) anionic species sorption onto surfactant-modified montmorillonite clay[J].Journal of Colloid and Interface Science,229(1):230-236
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Lagergren S.1898.About the theory of so-called adsorption of soluble substances[J].Kungliga Svenska Vetenskapsakademies Handlingar,24(4):1-39
Langmuir I.1918.The adsorption of gases on plane surfaces of glass,mica and platinum[J].Journal of the American Chemical Society,40(9):1361-1403
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Lim Y S,Kim K H.2017.Isotherm,kinetic and thermodynamic studies on the adsorption of 13-dehydroxybaccatin III from Taxus chinensis onto Sylopute[J].The Journal of Chemical Thermodynamics,115:261-268
Liu G H,Zhang Z H,Yan C,et al.2018.Adsorption of estrone with few-layered boron nitride nanosheets:Kinetics,thermodynamics and mechanism[J].Chemosphere,207:534-542
刘洪国,孙德军,郝京诚.2016.新编胶体与界面化学[M].北京:化学工业出版社
Schr?der M.2010.Functional Metal-Organic Frameworks:Gas Storage,Separation and Catalysis[M].Berlin Heidelberg:Springer-Verlag
consideration of the correct calculation of thermodynamic parameters of adsorption[J].Journal of the Serbian Chemical Society,72(12):1363-1367
牛鹏举,魏世勇,方敦,等.2016.高岭石、针铁矿及其二元体对胡敏酸的吸附特性[J].环境科学,37(6):2220-2228
Rahimi E,Mohaghegh N.2016.Removal of toxic metal ions from sungun acid rock drainage using mordenite zeolite,graphene nanosheets,and a novel metal-organic framework[J].Mine Water and the Environment,35(1):18-28
Santos S,Ungureanu G,Boaventura R,et al.2015.Selenium contaminated waters:An overview of analytical methods,treatment options and recent advances in sorption methods[J].Science of the Total Environment,521-522:246-260
Schiavon M,Ertani A,Parrasia S,et al.2017.Selenium accumulation and metabolism in algae[J].Aquatic Toxicology,189:1-8
Song G Q,Wang Z Q,Wang L,et al.2014.Preparation of MOF(Fe) and its catalytic activity for oxygen reduction reaction in an alkaline electrolyte[J].Chinese Journal of Catalysis,35(2):185-195
Sposito G.2008.The Chemistry of Soils(2nh ed)[M].New York:Oxiford University Press
Tran H N,You S J,Chao H P.2016.Thermodynamic parameters of cadmium adsorption onto orange peel calculated from various methods:A comparison study[J].Journal of Environmental Chemical Engineering,4(3):2671-268
Tran H N,You S J,Hosseini-Bandegharaei A,et al.2017.Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions:A critical review[J].Water Research,120:88-116
Walter W J.1984.Evolution of a Technology[J].Journal of Environmental Engineering,110(5):899-917
王锐,许海娟,魏世勇,等.2018a.MOF-Fe吸附Se(Ⅳ)的特性与机制研究[J].环境科学学报,38(8):3127-3137
王锐,龚勇,许海娟,等.2018b.不同调节剂制备MOF-Fe的性质及对Se(Ⅳ)的吸附性能[J].无机化学学报,34(5):906-916
Weber W J,Morris J C.1963.Kinetics of adsorption on carbon from solution[J].Journal of the Sanitary Engineering Division,89:31-60
Winkel L H,Johnson C A,Lenz M,et al.2011.Environmental selenium research:from microscopic processes to global understanding[J].Environmental Science & Technology,46(2):571-579
Zhao H S,Robert S.2001.Competitive adsorption of phosphate and arsenate on goethite[J].Environmental Science & Technology,35(24):4753-4757
Arai Y,Sparks D L.2001.ATR-FTIR spectroscopic investigation on phosphate adsorption mechanisms at the ferrihydrite-water interface[J].Journal of Colloid and Interface Science,241(2):317-326
Blanchard G,Maunaye M,Martin G.1984.Removal of heavy metals from waters by means of natural zeolites[J].Water Research,18(12):1501-1507
Constantino L V,Quirino J N,Monteiro A M,et al,2017.Sorption-desorption of selenite and selenate on Mg-Al layered double hydroxide in competition with nitrate,sulfate and phosphate[J].Chemosphere,181:627-634
Fernández-Martínze A,Charlet L.2009.Selenium environmental cycling and bioavailability:a structural chemist point of view[J].Reviews in Environmental Science and Bio/Technology,8(1):81-110
Freitas A F,Mendes M F,Coelho G L V.2007.Thermodynamic study of fatty acids adsorption on different adsorbents[J].The Journal of Chemical Thermodynamics,39(7):1027-1037
Freundlich H M F.1906.Uber die adsorption in lasungen[J].Journal of Physical Chemistry,57:385-470
Guesh K,Caiuby C A D,Mayoral á,et al.2017.Sustainable preparation of MIL-100(Fe) and its photocatalytic behavior in the degradation of methyl orange in water[J].Crystal Growth & Design,17(4):1806-1813
Guo X,Feng Y R,Ma L,et al.2017.Phosphoryl functionalized mesoporous silica for uranium adsorption[J].Applied Surface Science,402:53-60
国家环境保护总局.2002.GB 3838-2002 地表水环境质量标准[S].北京: 国家质量监督检验检疫总局
Holmes A B,Gu F X.2016.Emerging nanomaterials for the application of selenium removal for wastewater treatment[J].Environmental Science-Nano,3(5):982-996
Howarth A J,Katz M J,Wang T C,et al.2015.High efficiency adsorption and removal of selenate and selenite from water using metal-organic frameworks[J].Journal of the American Chemical Society,137(23):7488-7484
Ju W,Li X,Li Z,et al.2017.The effect of selenium supplementation on coronary heart disease:A systematic review and meta-analysis of randomized controlled trials[J].Journal of Trace elements in Medicine and Biology,44:8-16
Jun J W,Tong M M,Jung B K,et al.2015.Effect of central metal ions of analogous metal-organic frameworks on adsorption of organoarsenic compounds from water:Plausible mechanism of adsorption and water Purification[J].Chemistry - A European Journal,21(1):347-354
Khare N,Martin J D,Hesterberg D.2007.Phosphate bonding configuration on ferrihydrite based on molecular orbital calculations and XANES fingerprinting[J].Geochimica et Cosmochimica Acta,71(18):4405-4415
Krishna B S,Murty D S R,Jai Prakash B S.2000.Thermodynamics of chromium(VI) anionic species sorption onto surfactant-modified montmorillonite clay[J].Journal of Colloid and Interface Science,229(1):230-236
Kumar P,Pournara A,Kim K H,et al.2017.Metal-organic frameworks:Challenges and opportunities for ion-exchange/sorption applications[J].Progress in Materials Science,86:25-74
Lagergren S.1898.About the theory of so-called adsorption of soluble substances[J].Kungliga Svenska Vetenskapsakademies Handlingar,24(4):1-39
Langmuir I.1918.The adsorption of gases on plane surfaces of glass,mica and platinum[J].Journal of the American Chemical Society,40(9):1361-1403
Li J,Wang X X,Zhao G X,et al.2018.Metai-organic framework-based materials:Superior adsorbents for the capture of toxic and radioactive metal ions[J].Chemical Society Reviews,47(7):2322-2356
Lim Y S,Kim K H.2017.Isotherm,kinetic and thermodynamic studies on the adsorption of 13-dehydroxybaccatin III from Taxus chinensis onto Sylopute[J].The Journal of Chemical Thermodynamics,115:261-268
Liu G H,Zhang Z H,Yan C,et al.2018.Adsorption of estrone with few-layered boron nitride nanosheets:Kinetics,thermodynamics and mechanism[J].Chemosphere,207:534-542
刘洪国,孙德军,郝京诚.2016.新编胶体与界面化学[M].北京:化学工业出版社
Schr?der M.2010.Functional Metal-Organic Frameworks:Gas Storage,Separation and Catalysis[M].Berlin Heidelberg:Springer-Verlag
consideration of the correct calculation of thermodynamic parameters of adsorption[J].Journal of the Serbian Chemical Society,72(12):1363-1367
牛鹏举,魏世勇,方敦,等.2016.高岭石、针铁矿及其二元体对胡敏酸的吸附特性[J].环境科学,37(6):2220-2228
Rahimi E,Mohaghegh N.2016.Removal of toxic metal ions from sungun acid rock drainage using mordenite zeolite,graphene nanosheets,and a novel metal-organic framework[J].Mine Water and the Environment,35(1):18-28
Santos S,Ungureanu G,Boaventura R,et al.2015.Selenium contaminated waters:An overview of analytical methods,treatment options and recent advances in sorption methods[J].Science of the Total Environment,521-522:246-260
Schiavon M,Ertani A,Parrasia S,et al.2017.Selenium accumulation and metabolism in algae[J].Aquatic Toxicology,189:1-8
Song G Q,Wang Z Q,Wang L,et al.2014.Preparation of MOF(Fe) and its catalytic activity for oxygen reduction reaction in an alkaline electrolyte[J].Chinese Journal of Catalysis,35(2):185-195
Sposito G.2008.The Chemistry of Soils(2nh ed)[M].New York:Oxiford University Press
Tran H N,You S J,Chao H P.2016.Thermodynamic parameters of cadmium adsorption onto orange peel calculated from various methods:A comparison study[J].Journal of Environmental Chemical Engineering,4(3):2671-268
Tran H N,You S J,Hosseini-Bandegharaei A,et al.2017.Mistakes and inconsistencies regarding adsorption of contaminants from aqueous solutions:A critical review[J].Water Research,120:88-116
Walter W J.1984.Evolution of a Technology[J].Journal of Environmental Engineering,110(5):899-917
王锐,许海娟,魏世勇,等.2018a.MOF-Fe吸附Se(Ⅳ)的特性与机制研究[J].环境科学学报,38(8):3127-3137
王锐,龚勇,许海娟,等.2018b.不同调节剂制备MOF-Fe的性质及对Se(Ⅳ)的吸附性能[J].无机化学学报,34(5):906-916
Weber W J,Morris J C.1963.Kinetics of adsorption on carbon from solution[J].Journal of the Sanitary Engineering Division,89:31-60
Winkel L H,Johnson C A,Lenz M,et al.2011.Environmental selenium research:from microscopic processes to global understanding[J].Environmental Science & Technology,46(2):571-579
Zhao H S,Robert S.2001.Competitive adsorption of phosphate and arsenate on goethite[J].Environmental Science & Technology,35(24):4753-4757
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