Research PaperSynthesis and adsorption properties of gelatin-conjugated hematite (α-Fe2O3) nanoparticles for lead removal from wastewater
Graphical Abstract
Introduction
Water pollution is the most serious environmental concerns, which can pose a direct risk to living creatures who may consume contaminated water. Heavy metals are regarded as one of the most hazardous water contaminants because they are nondegradable and accumulate in the body, causing serious issues such as brain disorders, anemia, kidney failure, and cancer (Xu et al., 2018, Riaz et al., 2020, Elgaml et al., 2019, Zeng et al., 2019). In particular, lead, one of ten substances which falls under the restriction of hazardous substances (RoHS) directive, is one of the most problematic materials in the world (Deubzer, 2019). Lead pollution is caused by the industrial manufacturing of materials such as metal plating, ammunition, ceramic, glass, and batteries. Recently, perovskite solar cells have taken the spotlight in the solar industry, owing to their unprecedented efficiency improvements. However, lead is a major component of perovskite materials (Park et al., 2020).
The Pb contaminated wastewater should be purified to less than 15 ppb as per the limitation of permissible levels and limits for lead in drinking or wastewater, provided by the World Health Organization (WHO) and Environmental Protection Agency (EPA). To purify Pb-contaminated wastewater, various methods such as chemical precipitation (Sun et al., 2020, Fu and Wang, 2011, Chen et al., 2018), reverse osmosis (Zhang et al., 2018, Li et al., 2017), ion exchange (Chen et al., 2017, Bashir et al., 2019, Dąbrowski et al., 2004), and surface adsorption (Hong et al., 2019, Baby et al., 2019, Maleki et al., 2016) have been investigated. The surface adsorption method, which uses metal oxide adsorbents, is the most efficient way to remove Pb ions because the process is economic, nontoxic, and simple. Recently, novel adsorbents such as doped metal oxides (Chen et al., 2019, Zou et al., 2018), nanostructured metal oxides (You et al., 2016, Sun et al., 2019), and the convergence of organic and metal oxides (Yilmaz et al., 2019) have been designed to enhance adsorption capacity and kinetics. For example, Co-doped Fe2O3 nanoparticles exhibited an improvement in adsorption capacity of 136 mg g−1 with an equilibrium time of 30 min (Chen et al., 2019). You et al (You et al., 2016). reported a hierarchically ordered Ca2SiO4 nanostructure that exhibited a high adsorption capacity of 458 mg g−1 with an equilibrium time of 2 h. It was reported more recently that polymer-grafted Fe3O4 nanoparticles can provide larger active sites by the surface functional groups, which exhibit a high Pb adsorption capacity of 129.65 mg g−1 with an equilibrium time of 108 min (Yilmaz et al., 2019). However, the recollection of metal oxide adsorbents is still challenging as well as adsorption performance.
In this study, we synthesized gelatin-conjugated hematite nanoparticles (HT NPs) with a small size of 4–6 nm by a novel and simple precipitation method, and investigated their adsorption capacity and kinetics for Pb removal. These gelatin-conjugated HT NPs exhibited simultaneous improvement of the adsorption capacity and kinetics. We found that the highly negative charge of HT NPs strengthens its reactivity with Pb, and the conjugated gelatin on the surface HT NPs provides a large number of active sites, such as amino and carboxyl groups, yielding a high purification performance, with a high adsorption capacity of 169.49 mg g−1 and a fast equilibrium time of 10 min
Section snippets
Materials
Iron(III) chloride hexahydrate (FeCl3∙6 H2O, 99%), urea (CH4N2O, 99.5%), gelatin (from bovine skin, Type B), sodium dihydrogen phosphate dehydrate (NaH2PO4∙2 H2O, 99%), sodium hydroxide (NaOH, 98%), sodium sulfate (Na2SO4, 99%), and sodium chloride (NaCl, 99.5%) were purchased from Sigma Aldrich. All chemical reagents were purchased and used without further purification.
Synthesis of iron oxide and hydroxide
Iron oxide and hydroxide were synthesized by simple precipitation under mild conditions. In a typical synthetic process,
Results and discussion
Iron oxide and hydroxide nanoparticles were synthesized via two different pathways by a simple precipitation method, as illustrated in Fig. 1(a). Ferrihydrite was precipitated as soon as the pH was increased to 13, and the precipitate exhibited a spherical nanoparticle (NP) with a small size of 4–6 nm. The NPs were then transformed into goethite and hematite by different phase transformation mechanisms with and without phosphate ions.
Fig. 1(b) shows the XRD patterns of the different crystal
Conclusion
In summary, we synthesized gelatin-conjugated HT NPs via a novel and simple precipitation method using a phosphate anion as a stabilizer. The phosphate ions retarded the dissolution and recrystallization of initial ferrihydrite, leading to a solid-state phase transition to spherical HT NPs with sizes of 4 nm to ~6 nm. The adsorption properties of the HT NPs were investigated for Pb ion removal from wastewater. We found that the highly negative charge of HT NPs led to the enhancement of the
CRediT authorship contribution statement
Hee Jung Kim: Conceptualization, Methodology, Formal analysis, Writing - original draft. Jae Myeong Lee: Investigation, Formal analysis, Methodology, Writing - review & editing. Jin Hyuk Choi: Investigation, Formal analysis. Dong Hoe Kim: Investigation, Methodology. Gill Sang Han: Conceptualization, Writing - review & editing, Supervision. Hyun Suk Jung: Funding acquisition, Writing - review & editing, Supervision.
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.
Acknowledgment
This work was supported by the Samsung Research Funding & Incubation Center of Samsung Electronics under Project Number SRFC-MA1901-07.
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These authors contributed equally to this work.