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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

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Front. Chem. Sci. Eng.    2015, Vol. 9 Issue (2) : 242-257    https://doi.org/10.1007/s11705-015-1513-7
RESEARCH ARTICLE
Interactions between nano-TiO2 particles and algal cells at moderate particle concentration
Mingyu LIN1,Yao Hsiang TSENG2,Chin-Pao HUANG1,*()
1. Department of Civil and Environmental Engineering, University of Delaware, Newark, DE 19716, USA
2. Department of Chemical Engineering, Taiwan University of Science and Technology, Taipei, Taiwan, China
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Abstract

Nano-sized titanium dioxide (nano-TiO2) has wide industrial applications and therefore considerable chances of exposure are created for human beings and ecosystems. To better understand the interactions between nano-TiO2 and aquatic organisms, we first studied TiO2 uptake by algae exemplified by Pseudokirchneriella subcapitata. P. subcapitata were exposed to nano-TiO2 in a series of concentrations and at various pH. TiO2 uptake was quantified using a sedimentation curve analysis technique. After exposure of algae to TiO2, the variation of zeta potential was measured and the morphology of algae-TiO2 aggregate was observed with scanning electron microscopy and the optical microscopy. The steady-state TiO2 uptake was found to be pH-dependent and the isotherms can be described well by Freundlich model. TiO2 deposited on algal surfaces causes the shift of pHzpc of TiO2-covered algae from that of algae toward that of TiO2. The attraction between TiO2-covered algal cells induces the agglomeration of algae and TiO2 and thus the formation of algae-TiO2 aggregates in the size of 12 to 50 μm. The 2-D fractal dimension of the aggregates is pH-dependent and ranges from 1.31 to 1.67. The theoretical analysis of the Gibbs energy of interaction indicates that both TiO2 uptake by algae and the formation of algae-TiO2 aggregate are influenced by the interaction between TiO2 particles.
Keywords nano-TiO2      Pseudokirchneriella subcapitata      algal cells      titanium dioxide uptake     
Corresponding Author(s): Chin-Pao HUANG   
Online First Date: 23 June 2015    Issue Date: 14 July 2015
 Cite this article:   
Mingyu LIN,Yao Hsiang TSENG,Chin-Pao HUANG. Interactions between nano-TiO2 particles and algal cells at moderate particle concentration[J]. Front. Chem. Sci. Eng., 2015, 9(2): 242-257.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-015-1513-7
https://academic.hep.com.cn/fcse/EN/Y2015/V9/I2/242
TiO2 concentration /(mg·L?1) Number concentration of TiO2 /# TiO2 per mL Number ratio of TiO2 to algae (T/A) /# TiO2 per algal cell
30 5.4 × 1011 3.0 × 105
50 9.1 × 1011 5.0 × 105
80 1.5 × 1012 8.0 × 105
100 1.8 × 1012 1.0 × 106
120 2.2 × 1012 1.2 × 106
130 2.4 × 1012 1.3 × 106
150 2.7 × 1012 1.5 × 106
Tab.1  The initial TiO2 concentrations expressed in different ways
Fig.1  An example of the sedimentation curve analysis. Conditions: pH= 4.2, initial TiO2 concentration= 80 mg/L. (a) The linear fit for type 3 after the separation of type 2 and type 3; (b) the linear fit for type 2 after the separation of type 1 and type 2; (c) the linear fit for type?1, (d) The turbidity data (Tmeasured) and the accumulated fitted sedimentation curves (T3, T2 + T3 and Ttotal)
Fig.2  Time constants for type 1, type 2 aggregates (algae-TiO2 aggregates), type 3 particles (free TiO2) and TiO2 particles at pH (a) 4.2, (b) 5.4, (c) 6.9 and (d) 7.3. At pH 7.3, the analysis of sedimentation curves shows that the slope of the linear fit for type 3 is close to zero. The same phenomenon was observed for TiO2 particles at pH 7.3
Fig.3  The calculated β versus the measured RH of TiO2 from DLS measurement. RH of 173, 177 and 228 nm was obtained at pH 4.2 and the 10, 30 and 30 mg/L of TiO2 concentration, respectively. RH of 886 nm was obtained at pH 5.4 and 30 mg/L of the TiO2 concentration. RH of 695 nm was obtained at pH 6.9 and 30 mg/L of TiO2 concentration
Fig.4  The predicted RHversus the measured RH. The shaded area represents the zone of the type 1 aggregates, which have the predicted RH above 70 μm. Type 2 aggregates have the predicted RH in the range of 10 and 70 μm
Fig.5  (a) The relationship of TiO2 adsorption density Γ and mixing time. (b) The relationship of ln (free TiO2 concentration) and mixing time. Conditions: pH= 6.9, initial TiO2 concentration= 120 mg/L and I= 1 mmol/L (NaCl)
Fig.6  The average TiO2 deposition density (Γ) was plotted over the free TiO2 concentration (C) at different pHs (4.2 to 7.3); F 4.2, F5.4, F6.9 and F7.3 are the fitted results of Freundlich model
pH KF /mL per algal cell nF
4.2 3.01×105 64.94
5.4 4.03×10–1 1.88
6.9 2.36×103 4.70
7.3 4.87×105 Infinity
Tab.2  The parameters in multilayer model and free energy calculation at each pH
Fig.7  The Gibbs energy of interaction as a function of the separation distance of an approaching TiO2 particles and the n-layer-TiO2-covered algal surface at pH= (a) 4.2, (b) 5.4, (c) 6.9 and (d) 7.3
Fig.8  The energy barrier, the parameter 1/nF in Freundlich model, and the representative TiO2 uptake (at about 8 × 1011 # TiO2 per mL of free TiO2 concentration), as a function of pH. The maximum of these three curves is all around pH 6.4
Fig.9  Zeta potential of pure algae, pure TiO2 and algae-TiO2 aggregates as a function of pH
Fig.10  SEM images: (a) algal cells in the absence of TiO2; (b) and (c) after exposure to TiO2 (102 mg/L of initial TiO2 concentration)
Fig.11  Optical microscopic images: (a) algal cells in the absence of TiO2; (b)?(d) after exposure to TiO2 (80 mg/L of initial TiO2 concentration). (b), (c) and (d) are obtained at pH 4.2, 5.4 and 9.2, respectively
Fig.12  D2 is the slope of (log A) versus (log l). R2 for the linear regression is 0.67, 0.70, 0.60 and 0.66 at pHs 4.2, 5.4, 6.9 and 7.3, respectively
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