Cu-Ca-Al-layered double hydroxide modified by itaconic acid as an adsorbent for anionic dye removal: Kinetic and isotherm study
Graphical abstract
Introduction
As a subgroup of inorganic layered nanomaterials, layered double hydroxides (LDHs) are ionic lamellar mixed hydroxides that consisted of positively charged main layers and an interlayer region with charge-compensating anions undergoing anion-exchange chemistry [1]. They are generally demonstrated with a stoichiometry of [2]. In this formula, and represent divalent and trivalent metals of the layers, respectively, and is charge balancing anion in the interlayer region which can be readily replaced. Owing to their fantastic properties, nowadays LDHs with different compositions have received remarkable attention from academia and industry [3]. They are exhibited important properties such as ion exchange capability, acid-base properties, and adsorption capacity. They are also low-cost materials and their properties can be easily tailored. The use of these materials in drug delivery, catalysis, energy conversion and storage, environmental remediation, and sample preparation have been reported [4].
Despite the unique characteristics of LDHs, various functionalization strategies have been reported for the modification of LDHs to increase their performance and applications. Functionalization of LDHs can drastically improve their performance and properties. Until now, various functionalization strategies have been used for the modification of LDHs. Some common functionalization strategies included intercalation, hybrid assembly, surface modification, size and morphology regulation, layer composition tuning, and defect introduction which are discussed in detail in a reported review by Laipan et al [5]. Surface modification of nanoparticles with organic molecules bearing functional groups is a smart and common strategy to increase the adsorption capacity of adsorbents [6]. Due to its biodegradability and active functional groups (two carboxylic groups), itaconic acid (ITA) can play the role of a surface modifier [7]. More interestingly, it is reported that due to the ability of dicarboxylic acids to form a dianion (in the case of ITA, it can be converted to itaconate anion), these molecules can replace anions between layers of LDHs, which in turn increases the distance between the LDH layers [8].
As an important environmental concern in both developing and industrial countries, the lack of clean water due to the disposal of various toxic compounds into the environment caused drastic concerns about the creature’s health. Among the well-known pollutants, synthetic organic dyes are one of the important groups of water pollutants [9], [10]. The release of these contaminants is an increasing and serious global challenge from an environmental point of view. These relatively complex organic molecules are widely used in different industries such as leather tanning, food processing, paper making, cosmetics, textile, and plastics. As a water-soluble member of synthetic dyes, Congo red is used in a huge quantity in textile and biochemistry-based industries [11], [12]. It is a benzidine-based anionic dye that was discovered by Paul Bottinger in 1883. Generally, benzidine-based dyes are toxic and highly carcinogenic. Congo red is known to metabolize to benzidine, which is a carcinogen and mutagen compound for humans.
Until now, various decontamination techniques have been adopted to remove toxic compounds especially synthetic organic dyes from environmental media in both industrial and municipal wastewaters. Among the treatment techniques, the adsorption strategy provided a simple, low cost, and relatively fast methodology with high efficiency [13]. This conventional strategy is used in advanced wastewater treatment due to its ease of operation, and flexibility in adsorbent design. Recently, various synthetic and natural adsorbents including LDHs, mesoporous silica materials [14], metal-organic frameworks and their composites [15], [16], [17], [18], covalent organic polymers and their composites [19], [20], [21], and polysaccharide-based polymers [22] have been utilized as adsorbent materials for environmental applications like removal of pollutants from water. Notably, developing adsorbents with improved characteristics to be used for the adsorption process is an ongoing trend.
Herein, for the first time, we present the synthesis and characterization of a novel adsorbent of itaconic acid-modified Cu-Ca-Al LDH for adsorption purposes. To the best of our knowledge, this is the first report to study the potential application of itaconic acid-modified Cu-Ca-Al layered double hydroxide for adsorption purposes. To study the applicability of the prepared materials for adsorption purposes, Congo red as an anionic dye was selected to be removed from the aqueous solution. Kinetic studies were also conducted for the prepared materials.
Section snippets
Materials and methods
All materials were purchased from Sigma-Aldrich and Merck (Darmstadt, Germany). The stock standard solution of Congo red (2000 mg L−1) was prepared in water. Working standard solutions were prepared daily by diluting the stock solution. Deionized water was prepared by a lab-made water purification system.
Synthesis of Cu-Ca-Al-LDH
The Cu-Ca-Al-LDH was prepared according to the following procedure. At first, 976 mg of Cu(NO3)2·3H2O (4 mmol), 954 mg of Ca(NO3)2·4H2O (4 mmol), and 1.532 g of Al(NO3)3·9H2O (4 mmol) were
Synthesis of the materials
In this study, Cu-Ca-Al-LDH was prepared in a simple strategy. For the modification of the prepared LDH, ITA was applied. Due to their ability to establish a hydrogen bond between surface hydroxyl groups on the surface of the LDH and functional groups of organic dyes, as well as their ion exchangeability, LDH-ITA can be used as adsorbents to remove organic dyes from aqueous media. This molecule also has the advantage of biodegradability, which is a very important factor in the design of a green
Conclusions
In conclusion, the novel LDH-ITA nanoparticles were synthesized through an environmentally friendly synthetic approach by using ITA as a biodegradable surface modifier. Owing to its hydroxyl and carboxyl groups, the prepared LDH-ITA was applied as a novel adsorbent for the adsorption of Congo red from water. Carbon binds to the Cu-CA-Al-LDH surface through hydrogen bonding and also penetrates Cu-CA-Al-LDH layers as itaconate anions, replacing the anions between the pure Cu-CA-Al-LDH layers to
CRediT authorship contribution statement
Shirin Shabani: Software, Visualization, Writing – original draft, Conceptualization, Validation, Formal analysis, Investigation. Mohammad Dinari: Supervision, Project administration, Conceptualization, Validation, Investigation, Resources, Writing – review & editing.
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.
Acknowledgement
The authors wish to thank the research council of the Isfahan University of Technology.
References (38)
- et al.
Environmentally-friendly and ultrasonic-assisted preparation of two-dimensional ultrathin Ni/Co-NO3 layered double hydroxide nanosheet for micro solid-phase extraction of phenolic acids from fruit juices
Ultrason. Sonochem.
(2018) - et al.
Layered double hydroxides as the next generation inorganic anion exchangers: Synthetic methods versus applicability
Adv. Colloid Interface Sci.
(2017) - et al.
Preparation and characterization of poly (itaconic acid)-grafted crosslinked chitosan nanoadsorbent for high uptake of Hg2+ and Pb2+
Int. J. Biol. Macromol.
(2017) - et al.
Recent advances in metal-organic framework membranes for water treatment: A review
Sci. Total Environ.
(2021) - et al.
Recent advances in nanoscale zero-valent iron-based materials: Characteristics, environmental remediation and challenges
J. Clean. Prod.
(2021) - et al.
Synthesis, characterization and adsorbing properties of hollow Zn-Fe2O4 nanospheres on removal of Congo red from aqueous solution
Desalination
(2011) - et al.
Novel diamino-functionalized fibrous silica submicro-spheres with a bimodal-micro-mesoporous network: Ultrasonic-assisted fabrication, characterization, and their application for superior uptake of Congo red
J. Mol. Liq.
(2019) - et al.
Synthesis of hierarchical micro-mesoporous LDH/MOF nanocomposite with in situ growth of UiO-66-(NH2)2 MOF on the functionalized NiCo-LDH ultrathin sheets and its application for thallium (I) removal
J. Mol. Liq.
(2021) - et al.
Zeolitic imidazolate framework-based nanomaterials for the capture of heavy metal ions and radionuclides: A review
Chem. Eng. J.
(2021) - et al.
Impact of metal ions and organic ligands on uranium removal properties by zeolitic imidazolate framework materials
J. Clean. Prod.
(2021)
Initial behavior of intraparticle diffusion model used in the description of adsorption kinetics
Chem. Eng. J.
The Dubinin-Radushkevich equation and the underlying microscopic adsorption description
Carbon N. Y.
Removal of Congo Red from water by adsorption onto activated carbon prepared from coir pith, an agricultural solid waste
Dye. Pigment.
Adsorption characteristics of Congo Red onto the chitosan/montmorillonite nanocomposite
J. Hazard. Mater.
Kinetic study and equilibrium isotherm analysis of Congo Red adsorption by clay materials
Chem. Eng. J.
Synthesis of hierarchical Ni(OH)2 and NiO nanosheets and their adsorption kinetics and isotherms to Congo red in water
J. Hazard. Mater.
Adsorption of the anionic dye Congo red from aqueous solution onto natural zeolites modified with N, N-dimethyl dehydroabietylamine oxide
Chem. Eng. J.
Enhancement of the anionic dye adsorption capacity of clinoptilolite by Fe3+-grafting
J. Hazard. Mater.
Layered Double Hydroxides: Present and Future
Cited by (16)
Synthesis of porous calcium-guar gum benzoate nano-biohybrids for sorptive removal of congo red and phosphates from water
2023, International Journal of Biological MacromoleculesPreparation of low-cost and non-conventional macroalgae-based biosorbent for fast and effectively selective dye adsorption
2023, Materials Chemistry and Physics