Original ResearchComparison of Pb(II) and Cd(II) micro-interfacial adsorption on fine sediment in the Pearl River Basin, China
Introduction
More than 90% of heavy metals in river water bodies are enriched in sediment particles and transfer from the liquid-solid phase at the water-sediment particle exchange interface (Reczyński et al., 2020; Wang et al., 2019). Migration, transformation and interaction of pollutants on sediment surface have great influence on the aquatic environment (Fang et al., 2016; Huang et al., 2015; Wang et al., 2020). Heavy metal pollutants were deposited in bottom sediments along with sediment in the final step of aquatic environment migration in rivers and reservoirs (Michalski et al., 2013; Wang et al. 2015a). Heavy metals transported in the particulate phase or combined with suspended solids have a long residence time in river sediments (tens of thousands to thousands of years) (Lecce & Pavlowsky, 2014; Xie et al., 2014). Many studies have been undertaken to investigate the mechanism by which heavy metals are enriched in sediment and then migrate and transform with sediment in aquatic environments. Guan et al. (2016) considered that the static and turbulent conditions in aquatic environments would affect the transformation and migration of heavy metals on the sediment surface. Heavy metals on the sediment surface undergo adsorption and desorption in aquatic environments (Dang et al., 2015; Wang et al., 2014), and the adsorption and desorption reflected the occurrence and movement characteristics of heavy metals on sediment in aquatic environment. Generally, adsorption occurs when the concentration of heavy metals in the water phase is high, and desorption occurs when the concentration is low (Gao et al., 2014; Sun et al., 2015; Wang et al., 2019). The adsorption and desorption of heavy metals on the sediment surface are because of physical and chemical interactions (Crawford et al., 2017; Eldridge et al., 2015; Jalali & Moradi, 2013; Merloab et al., 2020). Most current studies have focused on the movement rule of heavy metals on sediment in the water bodies. However, the micro-interfacial mechanism of heavy metal adsorption on river sediment has not been systematically studied.
Isothermal and kinetics models are ordinarily used to study the interfacial interaction and kinetics characteristics of heavy metal adsorption by sediment particles. Isothermal adsorption models can also be used to describe the characteristics of the steady adsorption process. Bhattacharyya and Gupta (2007) have revealed the adsorption characteristics of Cd, Cu, Pb and other heavy metals on the acid-activated montmorillonite monolayer using isothermal model. Furthermore, Wang and Li (2014) have analyzed clay minerals using an isothermal adsorption equation to indicate the steady adsorption characteristics of Cu and Zn adsorption on sediment. Bourliva et al. (2015) selected the isothermal adsorption equation to simulate the experimental adsorption data of natural bentonite and Cd, Cu, Ni and Pb with natural bentonite. Thus, these researchers acquired the characteristic parameters of the adsorption process. Adsorption kinetics models such as pseudo-first-order, pseudo-second-order, and Elovich models were used to describe the observed adsorption kinetics. The liquid-film diffusion and intraparticle diffusion models were used to determine the rate-controlling step and time of each adsorption step. The pseudo-first-order kinetics model could describe the liquid-solid phase adsorption process based on the adsorption capacity (Ngambia et al., 2019). The pseudo-second-order model was used to analyze the chemisorption kinetics of the liquid phase (Mallakpour & Rashidimoghadam, 2019). The Elovich model could determine the initial adsorption rate and desorption constant (An et al., 2017). The liquid-film diffusion model was used to study the movement process of the adsorbate from the liquid phase to the solid phase (Malamis & Katasou, 2013). Whereas the intraparticle diffusion model was used to identify the pore diffusion mechanism of adsorption (Rajic et al., 2011). Oliveira et al. (2014) simulate the adsorption capacity of sediment using a pseudo-second-order model. Wang et al. (2016) have investigated the maximum theoretical adsorption capacity of humin on soil using a kinetics model to reveal the dynamic change in the adsorption process. Xu and Zhao (2013) have investigated the adsorption characteristics of the soil from southern China using isothermal and kinetics models. The results showed that the maximum theoretical adsorption capacity and adsorption activity of Pb and Cd on soil were particularly high. Chen and Zeng (2017) used isothermal and kinetics models to fit the experimental adsorption data of Cu ions on sediment, and they revealed the adsorption micro-interfacial characteristics of Cu ions on sediment. Thus, the adsorption characteristics of heavy metal ions such as Cd, Cu and Pb on sediment can be studied through the use of isothermal and kinetics models (Abdellaoui et al., 2019; Eldridge et al., 2015; Guan et al., 2019). Kumar et al. (2016) and Li et al. (2016a) analyzed the microscopic interfacial characteristics of pollutants on sediment, because they thought that the microscopic interfacial characteristics might be an important factor affecting adsorption. Micro-interfacial pattern recognition adsorption is generally divided into three steps: film diffusion, pore diffusion and an adsorption reaction at the active site (Igberase et al., 2018). Sen and Gomez (2011) applied the kinetics models of film diffusion and pore diffusion to the adsorption of Zn ions on natural bentonite, and they found that pore diffusion was not obvious during the early period, but gradually became the rate-controlling step upon further adsorption. Chen and Zeng (2017) investigated the dynamic adsorption process of Cu ions on sediment, and they found that film diffusion was used as the adsorption rate-controlling step during the early period. Pore diffusion was used as the adsorption rate-controlling step during the late period until an adsorption equilibrium was reached. Major studies have used isothermal models and kinetics models to reveal the micro-interfacial adsorption interaction of heavy metals on natural minerals. However, few studies have systematically investigated the micro-interfacial adsorption characteristics of heavy metals on sediment using isothermal, kinetics, film diffusion and intraparticle diffusion models. Meanwhile, the model parameters have not been comprehensively compared and discussed.
In this study, the meaning and range of the model parameter values of heavy metal (Pb and Cd) ions adsorption on sediment were discussed by using the theoretical isothermal, kinetics and micro-interfacial identification models. Langmuir, Freundlich and Temkin models were used to fit the isothermal experimental data, and the model parameters were analyzed and discussed. Moreover, the pseudo-first-order, pseudo-second-order and Elovich models were used to investigate the dynamic adsorption characteristics, and the model parameters were discussed. In addition, the film diffusion and intraparticle models were selected to analyze the experimental kinetics data, which determined the point in time of each adsorption rate-controlling step, and studied the controlling step of the micro-interfacial pattern recognition adsorption process.
Section snippets
Sampling
The sediment samples were collected from an estuary located at the intersection of the Lianhuashan Waterway and Shiziyang River in Panyu District, Guangzhou, Guangdong Province. The geographical coordinate of the sampling site was 22°58′54.3″N and 113°30′27.4″E. The Lianhuashan waterway is a tributary of the Pearl River system. The Shiziyang River is a drowned valley bay in the South China Sea and is located between the Dongjiang Estuary and the Pearl River Estuary. The 40 kg sediment samples
Isothermal adsorption characteristics
The adsorption capacity and strength constant KL of the Langmuir model parameters for Pb- and Cd-ion adsorption on sediment were analyzed, as shown in Fig. 2. When the concentration of Pb- and Cd-ion increased, the adsorption capacity increased, the slope of the model decreased, the intercept increased, qm increased, and KL decreased. The qm and KL values were stable after reaching a certain amount. Thus, when the solution concentration was 5 mg/L, the qm and KL values appeared the stable
Discussion
At present, little attention has been given to study the systematic application of isothermal and kinetics models for heavy metal ion adsorption on river sediment (Chen et al., 2009; Chen & Zeng, 2017). In this study, the micro-interfacial characteristics of Pb- and Cd-ion adsorption on river sediment were investigated by isothermal and kinetics adsorption experiments. The model parameter variations in the isothermal adsorption and adsorption kinetics processes were discussed in depth.
Conclusions
The isothermal, kinetics, film diffusion and intraparticle diffusion models were systematically used to reveal the steady and dynamic adsorption mechanisms of Pb- and Cd-ion on sediment in this study. This work discussed and summarized the actual meanings of the model parameters for the steady adsorption, dynamic adsorption and micro-interfacial pattern recognition of Pb- and Cd-ion. The main conclusions are as follows:
- (1)
The Langmuir, Freundlich and Temkin models of the isothermal models could
Declaration of competing interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work was supported by the National Natural Science Foundation of China (No.51879291). We express our gratitude to professor Huang Mingzhi of South China Normal University for providing experimental equipment. We acknowledge anonymous reviewers whose comments and suggestions greatly improved the paper.
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