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• Phosphate significantly enhanced GO transport in saturated porous media. • Enhanced role was due to electrostatic repulsion and deposition site competition. • Enhancement effect in goethite-coated sand was to a larger extent than that in sand. • Cation-bridging promoted the enhancement effects in the presence of Ca2+. In this study, transport behaviors of graphene oxide (GO) in saturated uncoated (i.e., clean sand) and goethite-coated sand porous media were examined as a function of the phosphate. We found that phosphate enhanced the transport of GO over a wide range of solution chemistry (i.e., pH 5.0–9.0 and the presence of 10 mmol/L Na+ or 0.5 mmol/L Ca2+). The results were mainly ascribed to the increase of electrostatic repulsion between nanoparticles and porous media. Meanwhile, deposition site competition induced by the retained phosphate was another important mechanism leading to promote GO transport. Interestingly, when the phosphate concentration increased from 0.1 to 1.0 mmol/L, the transport-enhancement effect of phosphate in goethite-coated sand was to a much larger extent than that in clean sand. The observations were primarily related to the difference in the total mass of retained phosphate between the iron oxide-coated sand and clean sand columns, which resulted in different degrees of the electrostatic repulsion and competitive effect of phosphate. When the background solution contained 0.5 mmol/L Ca2+, phosphate could be bind to sand/ goethite-coated sand surface by cation bridging; and consequently, promoted competition between phosphate and nanoparticles for deposition sites, which was an important mechanism for the enhanced effect of phosphate. Moreover, the DLVO theory was applicable to describe GO transport behaviors in porous media in the absence or presence of phosphate. Taken together, these findings highlight the important status and role of phosphate on the transport and fate of colloidal graphene oxide in the subsurface environment. [Display omitted] [ABSTRACT FROM AUTHOR]

In this study, batch and column tests were performed to investigate the co-transport of graphene oxide (GO) nanoparticles and tetracycline in saturated porous media under various solution chemistry conditions. Research indicated that GO and tetracycline had mutual promotion effect on their transport in the porous media under all the tested conditions, which was ascribed to the high adsorption capacity of tetracycline onto GO and the increased electrostatic repulsion as well as their competition for deposition sites on sand surfaces. Interestingly, the mutually promoting function of GO and tetracycline under acidic conditions was greater than that under alkaline conditions, the dominant mechanism was that the increased solution pH decreased the sorption of tetracycline onto GO and weakened the deposition site competition. Furthermore, the mutually promoting effect of GO and tetracycline was Na+ or Ca2+ concentration-dependent. Specially, increased Ca2+ concentration weakened the promoting effect of GO on tetracycline transport but magnified the promoting effect of tetracycline on GO transport. This is because higher Ca2+ concentration could cause a decrease in the adsorption of tetracycline on GO and facilitate more tetracycline molecules to occupy the deposition sites on sand surfaces. Additionally, sodium dodecyl sulfate had enhancement effect on co-transport of GO and tetracycline. Findings from this study clearly indicated that antibiotics and carbon based nanomaterials may transport together under various solution chemistry conditions, and consequently affect their fates in aquatic environments. Image 1 • GO and tetracycline have mutual promotion function on co-transport. • Sorption and deposition site competition contribute to mutually promoting effects. • Extent of tetracycline-mobilizing capability of GO depends on solution pH. • Different co-deposition mechanisms are involved in the presence of Ca2+ vs. Na+. • SDS has enhancement effect on co-transport of GO and tetracycline. GO and tetracycline had mutual promotion effect on their transport in the porous media under various solution chemistry conditions. [ABSTRACT FROM AUTHOR]

Since iron oxide minerals are ubiquitous in natural environments, the release of graphene oxide (GO) into environmental ecosystems can potentially interact with iron oxide particles and thus alter their surface properties, resulting in the change of their transport behaviors in subsurface systems. Column experiments were performed in this study to investigate the co-transport of GO nanoparticles and hematite colloids (a model representative of iron oxides) in saturated sand. The results demonstrated that the presence of hematite inhibited GO transport in quartz sand columns due to the formation of less negatively charged GO-hematite heteroaggregates and additional deposition sites provided by the adsorbed hematite on sand surfaces. Contrarily, GO co-present in suspensions significantly enhanced the transport of hematite colloids through different mechanisms such as the increase of electrostatic repulsion, decreased physical straining, GO-facilitated transport of hematite (i.e., highly mobile GO nanoparticles served as a mobile carrier for hematite). We also found that the co-transport behaviors of GO and hematite depended on solution chemistry (e.g., pH, ionic strength, and divalent cation (i.e., Ca2+)), which affected the electrostatic interaction as well as heteroaggregation behaviors between GO nanoparticles and hematite colloids. The findings provide an insight into the potential fate of carbon nanomaterials affected by mineral colloids existing in natural waters and soils. Image 1 • Hematite inhibited GO mobility by heteroaggregation and providing retention sites. • GO significantly enhanced hematite transport through multi-mechanisms. • Highly mobile GO acted as a carrier of hematite colloids. • Low pH or high ionic strength decreased the mobility of both particles. • Ca2+ magnified transport-enhancement effect of GO on hematite transport. [ABSTRACT FROM AUTHOR]

Humic acid (HA), a naturally occurring and widely distributed natural organic matter in the environment, is one of the most important factors controlling the transport and fate of mineral colloids. This study examined the influence of HA (0–10 mg/L) on the transport of goethite and hematite colloids in saturated quartz sand-packed columns under various solution chemistry conditions (including ionic strength and pH). We found that the transport-enhancement effect of HA on goethite colloids was greater than that on hematite colloids because the steric hindrance and electrostatic repulsion between HA-bound goethite colloids and sand stronger than those between HA-bound hematite colloids and sand. Besides, Ca2+ could be a bridging agent between HA and sand; and consequently, enhanced the steric hindrance between iron oxide colloids and sand, which was an important mechanism for the transport-enhancement effect of HA in the presence of Ca2+. Interestingly, with increasing HA concentration from 3 to 10 mg/L, the transport-enhancement effect of HA at higher ionic strength (i.e., 20 mM NaCl) was to a larger extent than that at lower ionic strength (i.e., 5 mM NaCl); meanwhile, the enhancement effect of HA at lower pH (i.e., 5.0) was to a larger extent than that at higher pH (i.e., 9.0). The observations were attributable to the surface charge and aggregation properties of HA-bound iron oxide colloids affected by solution chemistry coupled with HA concentration. Furthermore, DLVO theory extended by steric repulsion (XDLVO) could explain the observed trend of colloid transport under the test conditions. [ABSTRACT FROM AUTHOR]

Biomass-pyrogenic smoke-derived dissolved organic matter (SDOMs) percolating into the underground environment profoundly impacts the transport and fate of environmental pollutants in groundwater systems. Herein, SDOMs were produced by pyrolyzing wheat straw at 300–900 °C to explore their transport properties and effects on Cu2+ mobility in quartz sand porous media. The results indicated that SDOMs exhibited high mobility in saturated sand. Meanwhile, the mobility of SDOMs was enhanced at a higher pyrolysis temperature due to the decrease in their molecular sizes and the declined H-bonding interactions between SDOM molecules and sand grains. Furthermore, the transport of SDOMs was elevated as pH values were raised from 5.0 to 9.0, which resulted from the strengthened electrostatic repulsion between SDOMs and quartz sand particles. More importantly, SDOMs could facilitate Cu2+ transport in the quartz sand, which stemmed from forming soluble Cu–SDOM complexes. Intriguingly, the promotional function of SDOMs for the mobility of Cu2+ was strongly dependent on the pyrolysis temperature. Generally, SDOMs generated at higher temperatures exhibited superior effects. The phenomenon was mainly due to the differences in the Cu-binding capacities of various SDOMs (e.g., cation-π attractive interactions). Our findings highlight that the high-mobility SDOM can considerably affect heavy metal ions' environmental fate and transport. [Display omitted] • SDOMs exhibited excellent mobility in quartz sand over the pH range of 5.0–9.0 • The molecular sizes of SDOMs and H-bonding interactions contributed to the mobility. • SDOMs facilitated Cu2+ mobility owing to the formation of soluble SDOM-Cu complexes. • The promotion effects of SDOMs strongly depended on the pyrolysis temperature. [ABSTRACT FROM AUTHOR]

Water-soluble aerosol organic matters (WSAOMs) produced by biomass pyrolysis/burning can penetrate subsurface environment, and are anticipated to have a profound effect on the fate of contaminants in aquatic ecosystems. Herein, WSAOMs derived from corn straw (CS-WSAOMs) and pinewood sawdust (PW-WSAOMs) pyrolysis at 300–900 °C were utilized to investigate their mobility characteristics and impacts on the transport of heavy metal ions (i.e., Cd2+) in saturated quartz sand with or without soil colloids. This study clearly demonstrated that WSAOMs in subsurface systems exhibited high mobility, which increased as WSAOMs molecular sizes decreased and hydrogen-bond interactions between WSAOMs and sand grains declined. WSAOMs significantly improved heavy metal (i.e., Cd2+) and soil colloid-mediated Cd2+ mobility in the porous media, which stemmed from the increased binding affinities of colloids toward metal ions and the high mobility of WSAOMs. Interestingly, in terms of the mobility and colloid-facilitated transport of Cd2+, WSAOMs from higher pyrolysis temperatures exhibited enhanced effects; meanwhile, the PW-WSAOMs demonstrated stronger effects than the CS-WSAOMs. The trends were mainly attributed to the differences in the metal-binding affinities (e.g., cation-π interactions) and transport abilities of WSAOMs, as well as diverse Cd2+ adsorption capacities of colloids induced by various WSAOMs. [Display omitted] • WSAOMs exhibited high mobility in saturated quartz sand porous media. • The components and molecular sizes of WSAOMs strongly affect their transport. • WSAOMs enhanced Cd2+ mobility due to the formation of WSAOMs-metal complexes. • WSAOMs promoted soil colloid-facilitated transport of Cd2+ through multi-mechanisms. • Enhanced effects of WSAOMs depended on the biomass type and pyrolysis temperature. [ABSTRACT FROM AUTHOR]

Environment-ubiquitous low - molecular-weight organic acids (LMWOAs) can interact with heavy metal ions and thus affect their mobility in subsurface aquifers. Herein, the effects of LMWOAs (including acetic acid, tartaric acid, malonic acid, oxalic acid, and citric acid) on the mobility of heavy metal ions (including Cd2+, Zn2+, Ni2+, Mn2+, and Co2+) in porous media were investigated to reveal the role of the stability constants of metal-LMWOA complexes in the mobility of heavy metal ions in porous media. The results showed that the mobility of different metal ions followed the order of Cd2+ < Zn2+ < Ni2+ < Mn2+ < Co2+ despite of LMWOAs-free or LMWOAs-addition. For each heavy metal, all the organic acids enhanced its transport by forming stable non-adsorbing metal-LMWOA complexes and the enhanced ability followed the order of citric acid > oxalic acid > malonic acid > tartaric acid > acetic acid. An interesting finding was that there was a significantly positive correlation between the enhanced abilities of LMWOAs to metal mobility and the complex stability constants (log K) (R 2 = 0.801–0.961, p < 0.05), indicating that the complex stability of metal-LMWOA was the dominant factor responsible for the enhanced transport of heavy metal ions. Meanwhile, the linear slope indicated the intensity of enhancement of LMWOAs on heavy metal mobility was heavy metal type-dependent. This study proposed that the complex stability of metal-LMWOA could be an indicator to quantify and predict the impact of LMWOAs on the mobility of heavy metals. [Display omitted] • LMWOAs facilitate metal mobility due to the formation of non-adsorbing complexes. • For a given metal ion, the extent of enhanced effects depends on LMWOA species. • The complex stability is the dominant factor responsible for the enhanced effects. • The intensity of enhanced effects of LMWOAs on metal mobility depends on metal type. [ABSTRACT FROM AUTHOR]

Given the ubiquitous mineral (e.g., clays and iron oxides) playing critical roles in impacting the fate of antibiotics in the subsurface environment, the effects of two mineral colloids (i.e., ferrihydrite and montmorillonite) on tetracycline (TC, a representative of antibiotic) transport in sand columns were investigated in this study. Interestingly, the results clearly showed that ferrihydrite colloids inhibited TC transport, while montmorillonite colloids enhanced TC mobility under neutral conditions (pH 7.0). This phenomenon resulted from the positively charged ferrihydrite colloids with weak mobility, which assisted TC deposition; besides, providing additional deposition sites for TC by the deposited ferrihydrite colloids was another important mechanism. In contrast, the transport-enhancement effect of montmorillonite on TC was attributed to the strong binding affinity of TC to clay particles as well as the competition between colloids and TC for deposition sites on sand surfaces. Moreover, the transport-inhibition effect of ferrihydrite at pH 7.0 was greater than that at pH 5.0, mainly due to more colloid-associated TC under neutral conditions. Surprisingly, ferrihydrite colloids could act as carriers of antibiotics and enhanced TC transport at pH 9.0. Because the surface charge of colloids was altered to negative and could break through the column. Meanwhile, the transport-enhancement effect of montmorillonite decreased with increasing pH from 5.0 to 9.0, resulting from the decrease of colloid-adsorbed TC. Furthermore, colloid-mediated transport of TC was influenced by ionic strength, which affected the aggregation characteristics of colloids and the binding affinities of TC to minerals. These findings provide critical information for assessing the risks of antibiotics in aquatic ecosystems where abundant natural minerals are present. [Display omitted] • A comparison regarding the effect of iron oxide and clay on TC mobility was studied. • Ferrihydrite inhibited TC transport mainly due to colloid-associated TC deposition. • Providing additional sites by ferrihydrite was another deposition mechanism for TC. • Highly mobile montmorillonite acted as a carrier of TC and enhanced TC transport. • Colloid-mediated transport of TC considerably depended on solution chemistry. [ABSTRACT FROM AUTHOR]

Column experiments were carried out to investigate the transport of TiO 2 nanoparticles (n TiO 2) in water-saturated porous media in the presence of various imidazolium-based ionic liquids (ILs) with different alkyl chain lengths and counteranions. The results indicated that the effects of ILs on n TiO 2 transport were considerably dependent upon IL species. In general, the transport-inhibition effects increased with the increasing length of branched alkyl chain on the ILs (i.e., [C 6 mim]Cl > [C 4 mim]Cl > [C 2 mim]Cl). The trend was dominated by the hydrophobicity effects of ILs. Meanwhile, the inhibitory effects of ILs were strongly related to the counteranions and followed the order of [C 4 mim]Cl > [C 4 mim][TOS] > [C 4 mim][PF 6 ], mainly due to different electrostatic repulsion force between nanoparticles and porous media in the presence of various ILs. Furthermore, the inhibitory role of [C 4 mim][TOS] in n TiO 2 transport under acidic conditions (i.e., pH 6.5) was greater than that under alkaline conditions (i.e., pH 8.0). The dominant mechanism was that the differences in the extent of electrostatic repulsion between sand grains and n TiO 2 with or without ILs at pH 6.5 were larger than that at pH 8.0. Moreover, two-site kinetic retention model and DLVO theory provided good descriptions for the transport behaviors of n TiO 2 with different ILs. [Display omitted] • ILs significantly inhibit n TiO 2 transport in saturated porous media. • Transport-inhibition increases with increasing the length of branched alkyl chain. • Hydrophobic and electrostatic interactions dominate the transport of n TiO 2 with ILs. • Transport-inhibition effects of ILs are anion-dependent. [ABSTRACT FROM AUTHOR]