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Influence of fulvic acid on the colloidal stability and reactivity of nanoscale zero-valent iron
2016
Dong, Haoran | Ahmad, Kito | Zeng, Guangming | Li, Zhongwu | Chen, Guiqiu | He, Qi | Xie, Yankai | Wu, Yanan | Zhao, Feng | Zeng, Yalan
This study investigated the effect of fulvic acid (FA) on the colloidal stability and reactivity of nano zero-valent iron (nZVI) at pH 5, 7 and 9. The sedimentation behavior of nZVI differed at different pH. A biphasic model was used to describe the two time-dependent settling processes (i.e., a rapid settling followed by a slower settling) and the settling rates were calculated. Generally, the settling of nZVI was more significant at the point of zero charge (pHpzc), which could be varied in the presence of FA due to the adsorption of FA on the nZVI surface. More FA was adsorbed on the nZVI surface at pH 5–7 than pH 9, resulting in the varying sedimentation behavior of nZVI via influencing the electrostatic repulsion among particles. Moreover, it was found that there was a tradeoff between the stabilization and the reactivity of nZVI as affected by the presence of FA. When FA concentration was at a low level, the adsorption of FA on the nZVI surface could enhance the particle stabilization, and thus facilitating the Cr(VI) reduction by providing more available surface sites. However, when the FA concentrations were too high to occupy the active surface sites of nZVI, the Cr(VI) reduction could be decreased even though the FA enhanced the dispersion of nZVI particles. At pH 9, the FA improved the Cr(VI) reduction by nZVI. Given the adsorption of FA on the nZVI surface was insignificant and its effect on the settling behavior of nZVI particles was minimal, it was proposed that the FA formed soluble complexes with the produced Fe(III)/Cr(III) ions, and thus reducing the degree of passivation on the nZVI surface and facilitating the Cr(VI) reduction.
Show more [+] Less [-]Influence of macromolecules on aggregation kinetics of diesel soot nanoparticles in aquatic environments
2019
Chen, Chengyu | Wei, Jingyue | Li, Jing | Duan, Zhihui | Huang, Weilin
Soot nanoparticles (SNPs) produced from incomplete combustion have strong impacts on aquatic environments as they eventually reach surface water, where their environmental fate and transport are largely controlled by aggregation. This study investigated the aggregation kinetics of SNPs in the presence of macromolecules including fulvic acid (FA), humic acid (HA), alginate polysaccharide, and bovine serum albumin (BSA, protein) under various environmentally relevant solution conditions. Our results showed that increasing salt concentrations induced SNP aggregation by suppressing electrostatic repulsion and that CaCl2 exhibited stronger effect than NaCl in charge neutralization, which is in agreement with the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The aggregation rates of SNPs were variously reduced by macromolecules, and such stabilization effect was the greatest by BSA, followed by HA, alginate, and FA. Steric repulsion resulting from macromolecules adsorbed on SNP surfaces was mainly responsible for enhancing SNP stability. Such steric repulsion appeared to be affected by macromolecular structure, as BSA having a more compact globular structure on SNP surfaces imparted long-range steric repulsive forces and retarded the SNP aggregation rate by 10–100 times. In addition, alginate was shown to enhance SNP aggregation by ∼10 times at high CaCl2 concentrations due to alginate gel formation via calcium bridging. The results may bear strong significance for the fate and transport of SNPs in both natural and controlled environmental systems.
Show more [+] Less [-]Characterization of colloid-size copper-based pesticide and its potential ecological implications
2019
Tegenaw, Ayenachew | Sorial, George A. | Sahle-Demessie, Endalkachew | Han, Changseok
The intensive use of Cu-based pesticides in agriculture could have an unintended impact on the ecosystems and human health via different exposure pathways. This paper presents the results of experiments involving colloidal stability, aggregation, and dissolution of Cu₂O commercial pesticide under various environmental conditions in view of ecological implications. The investigated pesticide contains ∼750 g kg⁻¹ Cu (75% weight of product), Cu₂O particles with sizes < 1 μm, and nominal size fraction of Cu₂O nanoparticles. The co-presence of Ca²⁺ (20 mM) and humic acid (HA, 15 mg L⁻¹) significantly modulates (p < 0.001) the colloidal stability and mobility of particles. The dissolution of Cu at pH 5.5 was about 85%, 90%, and 75% weight more than the dissolution of Cu at pH 7.0, pH 8.5, and pH 7.0 and pH 8.5 combined, respectively in all dispersions. However, increasing HA content from 0 to 15 mg L⁻¹ reduced the dissolution of Cu by 56%, 50%, and 40% weight at pH 5.5, 7.0, and 8.5, respectively. Thus, pH below 7.0 is a critical factor to control the dissolution and bioavailability of Cu that may pose ecotoxicity and environmental pollution, whereas pH above 7.0 and the presence of HA attenuate the pH effect. These findings provide insight into how the potential mobility and bioavailability of Cu is modulated by the water chemistry under various environmental scenarios and media.
Show more [+] Less [-]Aggregation of oxidized multi-walled carbon nanotubes: Interplay of nanomaterial surface O-functional groups and solution chemistry factors
2019
Xia, Tianjiao | Guo, Xuetao | Lin, Yixuan | Xinbo, | Li, Shunli | Yan, Ni | Zhu, Lingyan
The fast-growing production and application of carbon nanotube (CNT) materials in a variety of industrial products inevitably lead to their release to wastewater and surface water. CNT would experience oxidization in wastewater treatment plant due to the presence of large amount of disinfectants, such as H₂O₂ and O₃, which in turn affects the environmental fates and risks of CNT. In this study, oxidized CNT materials (O-CNTs) were prepared by treating CNT with H₂O₂/UV and O₃ (denoting as H₂O₂-CNT and O₃-CNT, respectively). A variety of characterizations indicated that oxygen containing groups were generated on CNT surface upon the oxidation, and the O/C ratio increased in the order of pristine CNT < H₂O₂-CNT < O₃-CNT. In the presence of Na⁺, K⁺ and Mg²⁺, the O-CNTs displayed better colloidal stability than the pristine CNT, and the stability increased with the oxidation degree (indicated by O/C ratio). This could be explained by the more negative surface charge and stronger hydrophilicity of the O-CNTs. Unexpectedly, in the presence of Ca²⁺, the most oxidized O₃-CNT exhibited the poorest colloidal stability. The abundant carboxyl groups in O₃-CNT provided effective binding sites for cation bridging effect through Ca²⁺ and led to stronger aggregation. Increasing pH was more favorable to disperse CNTs (both O-CNT and pristine CNT) in the presence of Na⁺, but much less effective in inhibiting the aggregation of O₃-CNT in presence of Ca²⁺. This could be explained by the stronger cation bridging effect due to enhanced deprotonation the –COOH groups at higher pH conditions. The calculated Hamaker constants of the CNTs decreased with the oxidation degree, implying that there was lower van der Waals force between the O-CNTs. The Derjaguin–Landau–Verwey–Overbeek (DLVO) calculation confirmed that O-CNTs had to overcome higher energy barrier and thus showed better colloidal stability than the pristine CNT in the presence of Na⁺.
Show more [+] Less [-]Environmental fate and risk of ultraviolet- and visible-light-transformed graphene oxide: A comparative study
2019
Gao, Yang | Ren, Xuemei | Zhang, Xiaodong | Chen, Changlun
Currently, there is little comparative data on the colloidal stability and the toxicity of ultraviolet (UV)- and visible-light (VL)-transformed graphene oxide (GO). In order to identify this knowledge gap, the physicochemical properties of UV/VL-transformed GO are investigated in detail. Attempts are made to correlate the physicochemical alterations of UV/VL-transformed GO to the observed changes in its colloidal properties and toxicity. The results show that both UV and VL irradiations induce the significant change in the color, UV–vis absorbance, morphology, surface charge, size, oxygen containing functional groups, total of carbon, and photoluminescence properties of GO. The photo-reaction behavior of GO under UV exposure is different from that under VL irradiation in terms of reaction rate, order, and extent. Finally, the UV and VL irradiations show different effects not only on the colloidal stability of GO in the City water and Dongpu Lake water, but also on the toxicity of GO to Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus bacteria. This study clearly shows how the environmental fate and risk of GO are modified by UV and VL irradiations.
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