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Frontiers of Environmental Science & Engineering

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Front. Environ. Sci. Eng.    2019, Vol. 13 Issue (5) : 79    https://doi.org/10.1007/s11783-019-1163-y
RESEARCH ARTICLE
Influence of phosphate on deposition and detachment of TiO2 nanoparticles in soil
Zhan Wang1,2, Chongyang Shen1, Yichun Du3, Yulong Zhang2, Baoguo Li1()
1. Department of Soil and Water Sciences, China Agricultural University, Beijing 100193, China
2. College of Land and Environment, Shenyang Agricultural University, Shenyang 110866, China
3. Key Laboratory of Degraded and Unused Land Consolidation Engineering, Ministry of Land and Resources, Shaanxi Provincial Land Engineering Construction Group Co., Ltd., Xi’an 710075, China
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Abstract

We examined influence of phosphate on transport of TiO2 NPs in soil.

Deposition was reduced at higher pH and by adsorption of phosphate in soil.

Release was more for NPs initially deposited at higher pH.

Release was more for NPs initially deposited in the presence of phosphate.

Surface roughness and charge heterogeneity play a role in the deposition/ release.

The widespread use of TiO2 nanoparticles (NPs) makes inevitable their release into the soil. Phosphate is also widespread within soil, and is likely copresent with TiO2 NPs. However, the influence of phosphate on deposition/release— and thereby on transport— of TiO2 NPs in soil is yet to be elucidated. In this study we conducted saturated column experiments to systematically examine the transport of TiO2 NPs in soil amended with phosphate at different ionic strengths (ISs) (1, 10, 100 mmol/L NaCl) and pHs (4 and 9). Results show that the deposition of TiO2 NPs decreased with decreasing IS, increasing pH, and when soil absorbed phosphate. These observations are qualitatively in agreement with Derjaguin-Landau-Verwey-Overbeek (DLVO) interaction energy calculations, because the repulsive energy barrier is larger and secondary minimum depth is smaller at a lower IS, higher pH, and in the presence of phosphate. Accordingly, both primary- and secondary-minimum deposition were inhibited. Interestingly, although the deposition was less at higher pH and in the presence of phosphate, the subsequent spontaneous detachment and detachment by reduction of solution IS in these cases were greater. In addition, the presence of phosphate in the solution can cause a small quantity of attached TiO2 NPs to detach, even without perturbations of physical and chemical conditions. Our study was the first to investigate the influence of phosphate on detachment of TiO2 NPs and the results have important implication for accurate prediction of fate and transport of TiO2 NPs in subsurface environments.
Keywords Phosphate      TiO2 nanoparticles      Transport      Soil      Deposition      Detachment     
Corresponding Author(s): Baoguo Li   
Issue Date: 09 October 2019
 Cite this article:   
Zhan Wang,Chongyang Shen,Yichun Du, et al. Influence of phosphate on deposition and detachment of TiO2 nanoparticles in soil[J]. Front. Environ. Sci. Eng., 2019, 13(5): 79.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-019-1163-y
https://academic.hep.com.cn/fese/EN/Y2019/V13/I5/79
pH TOC
(g/kg)		 DOC
(g/kg)		 CEC
(cmol/kg)		 Free iron oxides
(g/kg)		 Specific surface area
(m2/g)
5.70 7.569 0.212 14.10 17.63 63.45
Tab.1  Physical and chemical properties of soil. TOC, total organic carbon; DOC, dissolved organic carbon; CEC, cation exchange capacity. pH, TOC, free iron oxides, and specific surface area were measured by potentiometry, ammonium acetate exchange, sodium disulfite-sodium citrate-sodium bicharbonate, and saturated potassium acetate methods, respectively. TOC and DOC were measured by Elemental analyzer (Elementar Vario EL III, Germany) and TOC-1020A (Elementar, Germany), respectively
pH IS
(mmol/L)		 Phosphate
(mg/L)		 Zeta potentials of soil
(mV)		 Zeta potentials of NPs
(mV)		 Sizes of NPs
(nm)
9 1 50 -31.7 -34.5 1269.3
9 1 0 -28.7 -23.9 1513.3
9 10 50 -26.2 -31.8 1334.7
9 10 0 -25.9 -22.9 2589.3
9 100 0 -19.2 -10.9 2464.7
4 1 50 -21.4 -23.5 1281.0
4 1 0 -20.7 -18.2 1649.3
4 10 50 -25.1 -18.5 1604.0
4 10 0 -20.4 -17.1 2884.0
4 100 50 -16.5 -15.8 1807.0
4 100 0 -13.1 -12.3 2898.3
Tab.2  Zeta potentials of soil and TiO2 NPs and sizes of TiO2 NPs in the absence/presence of phosphate
Fig.1  Breakthrough curves for transport of TiO2 NPs in columns packed with soil with or without absorbed phosphate (P) at different solution pHs and ISs. Phase 1, deposition of NPs in NaCl solution in soil either with (circle) or without (square) adsorption of phosphate; Phase 2, elution with NaCl solution; Phase 3, elution with NaCl solution with either lower IS (circle) or phosphate (square). Detailed experimental conditions are given in Table 3.
Figures pH Background solution (12 h) Phase 1 (5 PVs) Phase 2 (5 PVs) Phase 3（7 PVs）
Fig. 1
(a1)		 9 1 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 1 mmol/L NaCl 0.1 mmol/L NaCl
Fig. 1(a1) 9 1 mmol/L NaCl TiO2 NP suspension 1 mmol/L NaCl 1 mmol/L NaCl+ 50 mg/L phosphate
Fig. 1(a2) 9 10 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 10 mmol/L NaCl 1 mmol/L NaCl
Fig. 1(a2) 9 10 mmol/L NaCl TiO2 NP suspension 10 mmol/L NaCl 10 mmol/L NaCl+ 50 mg/L phosphate
Fig. 1(a3) 9 100 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 100 mmol/L NaCl 10 mmol/L NaCl
Fig. 1(a3) 9 100 mmol/L NaCl TiO2 NP suspension 100 mmol/L NaCl 100 mmol/L NaCl+ 50 mg/L phosphate
Fig. 1(b1) 4 1 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 1 mmol/L NaCl 0.1 mmol/L NaCl
Fig. 1(b1) 4 1 mmol/L NaCl TiO2 NP suspension 1 mmol/L NaCl 1 mmol/L NaCl+ 50 mg/L phosphate
Fig. 1(b2) 4 10 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 10 mmol/L NaCl 1 mmol/L NaCl
Fig. 1(b2) 4 10 mmol/L NaCl TiO2 NP suspension 10 mmol/L NaCl 10 mmol/L NaCl+ 50 mg/L phosphate
Fig. 1(b3) 4 100 mmol/L NaCl+ 50 mg/L phosphate TiO2 NP suspension 100 mmol/L NaCl 10 mmol/L NaCl
Fig. 1(b3) 4 100 mmol/L NaCl TiO2 NP suspension 100 mmol/L NaCl 100 mmol/L NaCl+ 50 mg/L phosphate
Tab.3  Conditions of the column experiments
Fig.2  Isotherms for phosphate adsorption in soil having NaCl electrolyte solutions at different ISs and pHs.
Fig.3  Fourier transform infrared (FTIR) spectrum of soil.
Fig.4  Calculated DLVO interaction energies between a spherical TiO2 NP and a planar soil surface, both with or without adsorption of phosphate (P), at different ISs and pHs.
Fig.5  
pH IS
(mmol/L)		 Phosphate
(mg/L)		 Primary minimum depth (kT) Maximum energy barrier (kT) Secondary minimum
Depth (kT) Distance (nm)
9 1 50 220.77 990.1 1.93 83.46
9 1 0 273.88 581.1 2.13 72.86
9 10 50 118.62 507.06 10.11 18.66
9 10 0 168.29 302.64 10.88 17.26
9 100 0 351.58 N.A. N.A. N.A.
4 1 50 308.57 402.47 2.29 68.46
4 1 0 336.21 276.88 2.42 63.26
4 10 50 204.61 201.21 11.64 16.26
4 10 0 243.86 112.47 12.55 14.66
4 100 50 313.47 N.A. N.A. N.A.
4 100 0 394.38 N.A. N.A. N.A.
Tab.4  Calculated primary minimum, maximum energy barrier, and secondary minima between a TiO2 NP and a soil surface at different pHs and ISs. N.A., absence of maximum energy barrier or secondary minimum
Fig.6  A scanning electron microscope (SEM) image of a soil particle surface.
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