纳米氧化铝对菲的吸附
Sorption of phenanthrene on Al2O3 nanoparticles
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摘要: 为揭示菲在人工纳米氧化铝上的吸附行为及溶液化学条件对吸附的影响,采用批量平衡实验研究了两种纳米氧化铝对菲的吸附,并考察了pH、盐度和重金属离子(Ni2+)对吸附行为的影响.结果表明,两种纳米氧化铝对菲均具有一定的吸附能力,吸附数据可用Freundlich模型较好地拟合,lgKF值分别为1.15(α-Al2O3)和1.07(γ-Al2O3).α-Al2O3对菲的吸附呈线性(n=0.96±0.03),其主要机制是菲在材料表面临近水层中的分配作用,而γ-Al2O3对菲的吸附表现出明显的非线性(n=1.19±0.01),其吸附过程除分配作用外,还可能存在孔填充机制;纳米氧化铝的团聚程度对两者的吸附行为也有影响.酸性和碱性条件下纳米氧化铝对菲的吸附均大于中性条件,在低pH条件下,纳米氧化铝与菲之间的静电吸引起主要作用,而在高pH下,纳米颗粒表面净电荷增加,团聚体的粒径减小,从而提供更多可利用的比表面积而促进吸附.盐度增加至32‰使两种纳米氧化铝的lgKF由1.15和1.07提高到1.60和2.12,这主要归因于盐析作用.Ni2+的存在对两种纳米氧化铝吸附菲也有促进作用,主要是纳米氧化铝表面电势增加和阳离子-π作用的结果.Abstract: In order to explore the sorption behavior of phenanthrene (PHE) on engineered Al2O3 nanoparticles (NPs) and the influence of solution chemistry on PHE sorption, batch experiments were conducted using α-Al2O3 and γ-Al2O3 NPs under different solution pH, salinity, and heavy metal ion (Ni2+) concentrations. The results indicated that these two types of Al2O3 NPs possessed sorption capability for PHE. The sorption data fit the Freundlich model well, with lgKF of 1.15 and 1.07 for α-Al2O3 NPs and γ-Al2O3 NPs, respectively. Sorption isotherm on α-Al2O3 NPs was linear (n=0.96±0.03), indicating PHE partitioning into the vicinal water layer of the sorbent; while PHE sorption on γ-Al2O3 NPs was nonlinear (n=1.19±0.01), possibly because of the involvment of pore filling besides partitioning mechanism. Sorption on the two NPs was also influenced by the extent NPs aggregation. Sorption under acid and basic conditions was higher than that under neutral condition. When pH was low, the electrostatic attraction dominated PHE sorption onto Al2O3 NPs. When pH was high, the net charge of NPs increased, resulting in less aggregation and greater available surface area of NPs. The lgKF increased from 1.15 to 1.60 (for α-Al2O3NPs) and 1.07 to 2.12 (for γ-Al2O3NPs) as the salinity increased to 32‰. This can be attributed to the salt-out effect. The coexistence of Ni2+ facilitated PHE sorption, which could be due to the increase of surface potential of Al2O3 NPs and the cation-π interaction.
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Key words:
- nano-Al2O3 /
- phenanthrene /
- sorption /
- pH /
- salinity /
- metal ion
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[1] JOO S H, ZHAO D Y. Environmental dynamics of metal oxide nanoparticles in heterogeneous systems:A review[J]. Journal of Hazardous Materials, 2017, 322(15):29-47. [2] HE Y, ZENG F F, LIAN Z H, et al. Natural soil mineral nanoparticles are novel sorbents for pentachlorophenol and phenanthrene removal[J]. Environmental Pollution, 2015, 205:43-51. [3] LIAN F, XING B S. Black carbon (biochar) in water/soil environments:Molecular structure, sorption, stability, and potential risk[J]. Environmental Science & Technology, 2017, 51(23):13517-13532. [4] REN X H, SUN H W,WANG F, et al. The changes in biochar properties and sorption capacities after being cultured with wheat for 3 months[J]. Chemosphere, 2016, 144:2257-2263. [5] WANG J, CHEN B L, XING B S. Wrinkles and folds of activated graphene nanosheets as fast efficient adsorptive sites for hydrophobic organic contaminants[J]. Environmental Science & Technology, 2016, 50(7):3798-3808. [6] WANG H, ZHAO X L, HAN X J, et al. Effects of monovalent and divalent metal cations on the aggregation and suspension of Fe3O4 magnetic nanoparticles in aqueous solution[J]. Science of the Total Environment, 2017, 586(15):817-826. [7] PARK C M, CHU K H, HEO J, et al. Environmental behavior of engineered nanomaterials in porous media:A review[J]. Journal of Hazardous Materials, 2016, 309(15):133-150. [8] FANG J, SHAN X Q, WEN B. et al, Sorption and desorption of phenanthrene onto iron, copper, and silicon dioxide nanoparticles[J].Langmuir,2008, 24(19):10929-10935. [9] TIAN S Y, ZHANG Y D, SONG C Z, et al. Titanium dioxide nanoparticles as carrier facilitate bioaccumulation of phenanthrene in marine bivalve, ark shell (Scapharcas ubcrenata)[J]. Environmental Pollution, 2014,192:59-64. [10] SU Y H, ZHU Y G, SHENG G Y, et al. Linear adsorption of nonionic organic compounds from water onto hydrophilic minerals:Silica and alinmina[J]. Environmental Science & Technology, 2006, 40(20):6949-6954. [11] WANG X L, LU J L, XU M G, et al. Sorption of pyrene by regular and nanoscaled metal oxide particles:Influence of adsorbed organic matter[J]. Environmental Science & Technology, 2008, 42(19):7267-7272. [12] SU C M. Environmental implications and applications of engineered nanoscale magnetite and its hybrid nanocomposites:A review of recent literature[J]. Journal of Hazardous Materials,2017, 332:48-84. [13] YANG K J, CHEN B L, ZHU X Y, et al. Aggregation, adsorption, and morphological transformation of graphene oxide in aqueous solutions containing different metal cations[J]. Environmental Science & Technology, 2006, 50(20):11066-11075. [14] 翁诗甫. 傅里叶变化红外光谱分析[M].第二版. 北京:化学工业出版社,2010. WENG S F. Fourier transform infrared spectral analysis[M]. Edition Ⅱ. Beijing:Chemical Industry Press, 2007 (in Chinese). [15] LI Z Y, LIU Y S, YANG X, et al. Performance of mesoporoussilicas and carbon in adsorptive removal of phenanthrene as a typical gaseous polycyclic aromatic hydrocarbon[J]. Microporous and Mesoporous Materials, 2017, 239:9-18. [16] SCHWARZENBACH R P, GSCHWEND P M, IMBODEN D M. Environmental Organic Chemistry, 2nd ed[M]. New Jersey:John Wiley& Sons, 2004. [17] YAN Y P, KOOPAL L K, LI W, et al. Size-dependent sorption of myo-inositol hexakisphosphate and orthophosphate on nano-γ-Al2O3[J]. Journal of Colloid and Interface Science, 2015,451:85-92. [18] HUANG W L, SCHLAUTMAN M A, WALTER J, et al. A distributed reactivity model for sorption by soils and sediments. 5. The influence of near-surface characteristics in mineral domains[J]. Environmental Science & Technology, 1996, 30(10):2993-3000. [19] WANG X X, CHEN Z S, TAN X L, et al. Effect of pH, humic acid and addition sequences on Eu (Ⅲ) sorption onto γ-Al2O3 study by batch and time resolved laser fluorescence spectroscopy[J]. Chemical Engineering Journal, 2016, 287:313-320. [20] HUANG T D, SUI M H, YAN X, et al. Anti-algae efficacy of silver nanoparticles to microcystis aeruginosa:Influence of NOM, divalent cations, and pH[J]. Colloids and Surface A:Physicochemical and Engineering Aspects, 2016, 509:492-530. [21] ZHANG S J, SHAO T, BEKAROGLU S S, et al. Adsorption of synthetic organic chemicals by carbon nanotubes:Effects of background solution chemistry[J]. Water Research, 2010, 44(6):2067-2074. [22] TURNER A, RAWLING M C. The influence of salting out on the sorption of neutral organic compounds in estuaries[J]. Water Research, 2001, 35(18):4379-4389. [23] SOFLA S J, JAMES L A, ZHANG Y H, Insight into the stability of hydrophilic silica nanoparticles in seawater for enhanced oil recovery implications[J]. Fuel, 2018, 216:559-571. [24] 吴志坚,刘海宁,张慧芳. 离子强度对吸附影响机理的研究进展[J]. 环境化学,2010,29(6):997-1003. WU Z J, LIU H N, ZHANG H F. Research progress on mechanisms about the effect of ionic strength on adsorption[J]. Environmental Chemistry, 2010, 29(6):997-1003(in Chinese).
[25] WANG F, SUN H W, REN X H, et al. Effects of humic acid and heavy metals on the sorption of polar and apolar organic pollutants onto biochars[J]. Environmental Pollution. 2017, 231(1):229-236. -

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