Abstract
One of the best and most affordable ways to remove harmful metals from water is by adsorption. This study investigated the efficiency of guinea fowl (Numida meleagris) eggshells as a low-cost adsorbent for cadmium (Cd) and nickel (Ni) removal from landfill leachate. In replicas, 100 mL wastewater was added to each of the weighed adsorbent dosages (1 g, 1.5 g, 2 g, 2.5 g, 3.0 g, and 3.5 g) in a flat-bottom flask and agitated for 60 minutes at pH of 7.82 and temperature 24 °C. The adsorption efficacy of cadmium and nickel by guinea fowl eggshells were 90.5% to 96.5% and 96.1% to 99.3%, respectively. The maximum adsorption capacity of cadmium was 4.89 × 10-2 mg/g and an adsorption equilibrium (KL) 22.74 mg/L. The Langmuir isotherm model was better fitted to the results of the experiment than the Freundlich isotherm model.
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Adsorption of Toxic Metals from Landfill Leachate onto Guinea Fowl Eggshells in the Era of Green Chemistry
Abudu Ballu Duwiejuah,* Elijah Yinigani Ayine, and Joseph Payne
One of the best and most affordable ways to remove harmful metals from water is by adsorption. This study investigated the efficiency of guinea fowl (Numida meleagris) eggshells as a low-cost adsorbent for cadmium (Cd) and nickel (Ni) removal from landfill leachate. In replicas, 100 mL wastewater was added to each of the weighed adsorbent dosages (1 g, 1.5 g, 2 g, 2.5 g, 3.0 g, and 3.5 g) in a flat-bottom flask and agitated for 60 minutes at pH of 7.82 and temperature 24 °C. The adsorption efficacy of cadmium and nickel by guinea fowl eggshells were 90.5% to 96.5% and 96.1% to 99.3%, respectively. The maximum adsorption capacity of cadmium was 4.89 × 10-2 mg/g and an adsorption equilibrium (KL) 22.74 mg/L. The Langmuir isotherm model was better fitted to the results of the experiment than the Freundlich isotherm model.
DOI: 10.15376/biores.18.3.4519-4531
Keywords: Adsorption; Guinea fowl eggshells; Landfill leachate; Nickel; Wastewater
Contact information: Department of Biotechnology, Faculty of Biosciences, University for Development Studies, Tamale, Ghana;
* Corresponding author: aduwiejuah@uds.edu.gh
INTRODUCTION
Poor landfill management results in the production of toxic leachate, which has a substantial negative influence on the nearby freshwater and groundwater. The aqueous effluent produced by solid waste as a result of its physical, chemical, and biological modification in landfills is known as leachate. Among the several elements that make up landfill leachate, heavy metals are non-biodegradable, capable of lowering the quality of surface and groundwater, and hazardous to biological systems even at low concentrations (Parvin and Tareq 2021).
Pollution of natural water with toxic metals has increased due to the expansion of industrial growth and development (Agboola et al. 2021). This causes environmental problems, including risks to human health. Toxic metals are non-biodegradable and toxic, and their presence in wastewater is a significant cause for concern (Isa et al. 2020). Also, Cd2+ and Ni2+ are found in wastewater such as agricultural sources, electroplating, metallurgical, mining, tanneries, and painting (Sultana et al. 2022). Cd2+ and Ni2+ are accumulative and toxic even at low concentrations, and they are potentially carcinogenic to living organisms (Allaoui et al. 2021). Most toxic ions offer a substantial threat to human health, as they can lead to serious illnesses and a variety of disorders when consumed in excess.
The insufficient removal of the Cd2+ and Ni2+ during water treatment is another concern of the environment, and the efficiency of treatments employed by the industries makes it more problematic. Not all chemical and physical separation processes are efficient for removal of these contaminants from an aqueous solution (Ramos et al. 2022). The existing methods of treatments are costly and regularly end up generating secondary contaminants (Sultana et al. 2022). This prompts the need for effective processes and simple techniques that are economically viable, environmentally efficient, and do not generate secondary contaminants. Among these, the process of adsorption stands out owing to its low cost, adsorbate recovery possibility, and operational simplicity (Ramos et al. 2021).
It was in the early ‘90s that the concept of green chemistry was developed by the United States Environmental Protection Agency (US-EPA); this concept has attracted great attention (Mukherjee 2022). In the era of green chemistry, pollution control is achieved by methods and technologies that are eco-friendly, less costly, simple to use, and effective. The concept of green chemistry leads to the search for new technologies and processes that from the very beginning cut short or prevent environmental contamination by reducing the chemical wastes volumes and their toxicity, using inoffensive or safer materials (Mukherjee 2022). This science is presently in an explosive growth and developmental stage. Green chemistry has emerged as a novel avatar to solve environmental pollution in order to secure the future (Anastas and Williamson 1996). In summary, green chemistry aims to design, produce, and use efficient, safe, effective, and more ecologically benign chemical processes and products, leading to environmental pollution control.
Eggshells offer numerous advantages in the green chemistry concept as adsorbents. These include affordability, eco-friendliness, and not requiring special preparations. The manufacturing industry has a severe problem of high heavy metal concentrations in wastewater. Eggshells, which are generated by the food and poultry industries with approximately 110 billion tonnes global annual production, have been considered a waste that ends up in landfills (Jannat et al. 2022). Guinea fowl eggs are one of the most consumed and enjoyed foods mostly in Africa and especially in Northern Ghana. Despite the fact that guinea fowl are supposed to have originated in Africa, global production has grown quickly in recent years. Under semi-intensive conditions, guinea fowl can be successfully raised with little effort (Yildirim 2012). Guinea fowl eggshells is an unappreciated waste; when improperly disposed, it becomes a public health and environmental concern and can contribute to proliferation of harmful microbes (Ayodele et al. 2021).
Eggshell contains 90 to 98% calcium carbonate (CaCO3) (Setiawan et al. 2018; Jannat et al. 2022). It has been reported to contain 94% CaCO3, 4% organic matter, 1% magnesium carbonate, and 1% calcium phosphate by weight (Ahmad et al. 2012) making calcium more highly bioavailable for easier adsorption than the commercially available limestone (Setiawan et al. 2018; Jannat et al. 2022). Mammillary cores, which are organic aggregates rich in sulphated proteoglycans and are present on the outside of eggshells, have the potential to bind calcium and serve as places where calcite crystals develop (Peigneux et al. 2020). The eggshell potentially can be applied in recycling, including treatment of wastewater.
Eggshells have economic value as an adsorbent (Lee et al. 2022). Additionally, metal ions and other actinides from diluted water solution might be bound by eggshells (Chen et al. 2013). Aside the cuticle on the outside, a spongy layer, and an inner lamellar layer are all ceramic components that make up the eggshell’s distinctively three-layered structure (Lunge et al. 2012). Eggshells have a high calcium carbonate concentration, which potentially makes them a good adsorbent for the treatment of water and soils polluted by metallic ions (Lee et al. 2022). Eggshells therefore have emerged as a suitable candidate in the search for readily available, cost-effective, non-toxic, and versatile material as potential adsorbent to remove contaminants from water (Mittal et al. 2016).
Considerably toxic metals including arsenic, cadmium, chromium, copper, lead, manganese, and mercury could be removed using eggshells. Elabbas et al. (2016) explored the removal of Cr(VI) ions from wastewater using crushed hen eggshells. Baláž et al. (2015) examined a batch adsorption system of Cd(II) removal capacity in wastewater using crushed eggshell. Park et al. (2007) studied the comparative Cr and Cd removal from electroplating wastewaters.
The eggshell’s porosity makes it a desirable material to utilize as a green source of adsorbent. In the adsorption of toxic metals from landfill leachate, chicken eggshells, guinea fowl eggshells, groundnut husk, rice husk, and others may be used. In this study, guinea fowl eggshells were used as a low-cost and green source adsorbent for cadmium and nickel adsorption from landfill leachate.
EXPERIMENTAL
Leachate was collected from Gbahili landfill site in Tamale, Northern Region, Ghana. Samples were collected into polypropene bottles, labelled, and transported at ice temperature.
Guinea Fowl Eggshells Preparation
The eggshells obtained from guinea fowl hatcheries in Tamale, Ghana were washed in deionised water, broken into suitable pieces, and sun dried for 48 h. Broken eggshells were ground into powder using a mortar and pestle and sieved using a 100 µm mesh sieve.
Experimental Setup
The landfill leachate sample was filtered with Whatman filter paper and analysed for the cadmium and nickel concentrations. The pH of the leachate from the landfill was measured using pH meter. A dosage of 0.5 g of powdered guineafowl eggshells (adsorbent) was added to 100 mL of landfill leachate in a conical flask and agitated for 60 minutes using an orbital shaker (Rotabit orbital shaker with 20 rpm to 230 rpm rotational speed) at a speed of 50 rpm. Repeated experiments were done for 1 g, 1.5 g, 2 g, 2.5 g, 3.0 g, and 3.5 g adsorbent dosages at pH of 7.82 and a temperature of 24 °C. The adsorbent-landfill leachate solutions were filtered using Whatman filter paper (125 mm Ø) and transferred into a 35 mL plastic bottles.
Adsorption Efficiency of Guinea Fowl Eggshell of Cadmium and Nickel
The removal efficiency (i.e., adsorption capacity) was calculated as follows,
(1)
where Qe is the adsorption capacity, Co is the initial concentration of Cd or Ni, Ce is the final concentration of Cd or Ni after adsorption, M is the amount or dosage of guinea fowl eggshells, and V is the volume of the solution.
Adsorption Isotherm Modelling
Adsorption isotherm models were used to show the relationship in the equilibrium state between the amount of cadmium and nickel solution on guinea fowl eggshell. To represent monolayer adsorption with the adsorbent surface, the Langmuir isotherm has been used (Sikdar et al. 2020).
The Freundlich model has been used to represent adsorption on heterogeneous surfaces adsorbents (Jeppu and Clement 2012). Hence, the study aims to estimate the affinity, understand the adsorption mechanism and properties of adsorbent surface with the adsorbate, and analyse the experimental conditions and the adsorption capacity relation (Hu and Zhang 2019). The Langmuir isotherm (Eq. 2) and its linear form Eq. 3) were used as follows,
(2)
(3)
where qe denotes the quantity of metal ions (Cd and Ni) adsorbed per gram of the guinea fowl eggshell at equilibrium (mg/g), Ce denotes the adsorbate equilibrium concentration (mg/L), qm denotes the maximum monolayer coverage capacity (mg/g), KL denotes Langmuir constant (L/mg). The qm values were determined from the intercept and slope of the Langmuir plot of Ce versus qe.
The Langmuir isotherm model important features were computed in terms of equilibrium parameter RL, which is a dimensionless constant denoted as equilibrium parameter or separation factor, calculated as follows,
(4)
where Co denotes the adsorbate initial concentration. When the RL = 1 is linear, RL > 1 is considered to be unfavourable, RL = 0 is irreversible, and when 0 ˂ RL ˂ 1, adsorption is favourable (Ayawei et al. 2017).
The Freundlich isotherm model is usually applied to describe the adsorption features of the heterogeneous surface. The Freundlich isotherm linear equation was expressed as follows,
(5)
where Kf denotes the Freundlich constant (mg/g), qe denotes the amount of adsorbed metal gram of the guinea fowl eggshell at equilibrium (mg/g), Ce denotes the landfill leachate equilibrium concentration (mg/L), n denotes adsorption density, and 
denotes the adsorption intensity.
RESULTS AND DISCUSSION
Adsorption Efficiency of Toxic Metals by Guinea Fowl Eggshells in Landfill Leachate
Guinea fowl eggshells achieved cadmium adsorption efficiency of 90.51% to 96.49% at the different dosages (Table 1). The level of cadmium adsorption is attributed to the availability and number of vacant active sites due to varying pores and heterogeneous surface of the eggshells, which aided Cd adsorption. The availability and number of active sites can be enhanced by the dosage of adsorbent. Moreover, dosage and contact time of the adsorbent are a function of removal efficiency and materials cost (Londono-Zuluaga et al. 2019). It has been reported that the contact time necessary to achieve acceptable removal rate of heavy metal may vary from one minute (Rodríguez et al. 2012) to six hours (Sofiane and Sofia 2015). Guinea fowl eggshells possess irregular, porous, and rough surfaces, with granularity and a distribution of tubular holes. The pores contribute to the gas exchange between the interior and exterior environments (Rajoriya et al. 2021). By increasing the amount of surface area that can interact with the pollutants, this feature facilitates the adsorption process on the adsorbent. A study by Abatan et al. (2022) stated that Cd(II) adsorption increased from 44.0 to 71.4% and Cr(VI) from 44.8 to 61.0% when the dosage of adsorbent was increased in the range 5 to 25 g for each 100 mg/L of the solution. The efficiency of adsorption of the adsorbent in an inactive amount drops with increasing target concentration. A study also used 1.0 g of eggshell, which was sufficient to remove high fractions of 95.6% of Cr3+ and 99.8% of Cd2+ (Zonato et al. 2022). Kalmykova et al. (2008) observed that the efficiency of adsorption of cadmium was 97.3% on sphagnum peat for a concentration of 100 ppb and declined to 86.6% when the Cd concentration was increased to 5000 ppb, which caused the sites of adsorption to reach saturation. Also, adsorption efficiency dropped significantly when the initial ions concentration was increased from 10 to 80 mg/L; the likely reasons are the saturation of the adsorbent active sites on the surface and the repulsive electrostatic force between the aqueous solution and the metal ions on the surface (Hassan et al. 2020).
Adsorption efficiency for nickel was 96.1% to 99.3%. This suggests that inexpensive guinea fowl eggshells can be utilised as an effective adsorbent to remove nickel from landfill leachate. The process of Ni2+ adsorption using eggshells is reported to reach adsorption equilibrium within 80 min (De Angelis et al. 2017). Considerably toxic metals including arsenic, cadmium, chromium, copper, lead, manganese, and mercury could be removed using eggshells. In a single factor, at a 24 h reaction time, copper concentration of 25 mg/L, 10 mg of adsorbent dose, and at 25 °C temperature, the efficiencies of adsorption of eggshell with a membrane and eggshell at pH 5 were 90.5% and 95.2%, respectively whilst at pH 5.9 the eggshell membrane was 73.3% (Chou et al. 2023). Elabbas et al. (2016) explored Cr(VI) ions removal from wastewater using crushed hen eggshells. Baláž et al. (2015) examined a batch adsorption system of Cd(II) removal capacity in wastewater using crushed eggshell. Park et al. (2007) studied the comparative Cr and Cd removal from electroplating wastewaters. These studies report the effective removal of Cr and Cd using eggshell as adsorbent.
The initial ion concentration of an aqueous solution has a prominent effect on the process of adsorption, as an increase in this concentration results in an increase in the ion load of the species adsorbed (Hassan et al. 2020). Mezenner and Bensmaili (2009) and Hosseini et al. (2022) showed that adsorption involves reactions on the surface, and with the passage of time, the sites of adsorption on the surface of adsorbent gradually decrease. The surface repulsion effect prevents adsorption by empty residual sites of adsorption on the surface. Adsorption occurs quickly at the initial stage and slows down as the sites of adsorption decrease; thus, the time affects the rate of adsorption (Hosseini et al. 2022).
The pH value recorded was 7.82 and the temperature recorded was 24 °C for the toxic metals in landfill leachate. The ionic state of the functional groups in a biomaterial is influenced by the pH of a solution, and this relationship can be utilised to explain the adsorption of Cd and Ni. Insufficient focus has been placed on the concurrent effects of the pH level on the ionic species of metals that are found in the bulk solution. The dissociation constants associated with various types of acidic groups at adsorbent surfaces have received attention (Hubbe et al. 2011). At a pH more than 7, the surface will be mostly negative, favouring the connection of Cd2+ and Ni2+, which are cations. At low pH values, removal of metal is restricted due to domination by hydrogen ions. This trend is likely owing to the competition between hydrogen and metal ions on the sites of adsorption. Hydrogen ion adsorption limits the attraction of metals. According to Moubarik (2015) at low pH values the surface charge is positive hence the adsorption of Cd is electrically unfavourable. Higher pH increases the negative charges on the eggshell surface, thus attracting the Cd cations and allowing its adsorption. According to Annane et al. (2021), the adsorption process of Cd ions on eggshells was optimised based on the adsorbent dose, initial pH, concentration, and contact time until saturation of the active sites.
Table 1. Adsorption of Metals by Guinea Fowl Eggshells in Landfill Leachate
Langmuir Adsorption Isotherm for Guinea Fowl Eggshells
The Langmuir adsorption isotherm was used to describe how cadmium and nickel interacted with guinea fowl eggshell active sites (surface) in landfill leachate. The maximum monolayer coverage adsorption capacity of cadmium was 4.89 × 10-2 mg/g with an adsorption equilibrium (KL) of 22.74 mg/L (Table 2), which is related to the extent of interaction between the guinea eggshells surface (adsorption energy) and adsorbate. There is a strong interaction between the adsorbate and adsorbent if the KL value is large, and smaller KL value implies a weak interaction. The present study showed a weak interaction between the guinea eggshells and Cd, as the maximum monolayer coverage adsorption capacity was relatively small. The maximum adsorption capacity of Cd was less than 3.01, 3.80 and 10.37 reported by Zonato et al. (2022), Abatan et al. (2022) and Flores-Cano et al. (2013), respectively (Table 3). This present study showed 4.89 × 10-2 mg/g for cadmium and was lower than 11.10 mg/g reported by Naema and Omar (2019). This present study showed KL of 22.74 mg/l, which was higher than 1.13 mg/L reported by Naema and Omar (2019). The RL for cadmium was 0.19 with a coefficient of determination (R2) of 0.0369 (Fig. 1). The RL for cadmium was 0.19, which indicates the shape of the isotherm for adsorption by eggshells was favourable because the RL was less than 1 (Ayawei et al. 2017). The RL value for Cd adsorption was close to zero because Cd was present in the landfill leachate at a relatively high concentration.
For nickel, the maximum adsorption in the landfill leachate was 5.29 × 10-3 mg/g, with an adsorption equilibrium (KL) of -5.18 mg/L (Table 2). The present study showed a weak interaction between the guinea eggshells and Ni, as the maximum monolayer coverage adsorption capacity was relatively low. As a larger value indicates a strong interaction between the adsorbent (guinea fowl eggshell) and adsorbate (Ni), whereas a weak interaction suggests a smaller value of Langmuir constant (Tran et al. 2019). The present study showed a maximum adsorption capacity of 5.29 × 10-3 mg/g for nickel, which was lower than the 13.5 mg/g reported by Kristianto et al. (2019). The present study found 5.18 mg/L for KL which is lower than the 0.6 mg/L reported by Kristianto et al. (2019). The RL for nickel was -2.30 with a coefficient of determination (R2) of 0.7021 (Fig. 2). The calculated Langmuir separation factor (RL) was -2.30 for Ni, indicating that the Langmuir isotherm may not be suitable indicators of the process of adsorption. The RL negative values could be due to the low initial concentrations of metal in the industrial wastewater used.
Table 2. Adsorption Isotherm Modelling of the Results of Guinea Fowl Eggshell
Table 3. Results of Similar Adsorption Studies
Freundlich Adsorption Isotherm for Guinea Fowl Eggshells
The 1/n value obtained for cadmium was 0.01, whereas the KF (mg/g) value obtained for cadmium was 477. The N value obtained for cadmium was 100 (Table 2) and the R2 value for cadmium was -0.0277 (Fig. 3). For nickel, the 1/n value obtained was -0.03, the KF (mg/g) value was 894.95, the N value was -33.33 (Table 2) and the R2 value was 0.4792 (Fig. 4). A description of heterogeneous adsorbent surfaces and the exponentially scattered active sites and energies on them is explained by the Freundlich isotherm (Ayawei et al. 2017). The KF measures an adsorbent’s capability for adsorption. The KF recorded for the adsorption process was 477 and 895 for cadmium and nickel, respectively. The 1/n recorded for cadmium and nickel was 0.01 and -0.03, respectively, which indicates that the adsorption normal 1/n is less than 1 (Ayawei et al. 2017).
Fig. 1. Langmuir isotherm for the adsorption of cadmium in landfill leachate by guinea fowl eggshells
Fig. 2. Langmuir isotherm for the adsorption of nickel in landfill leachate by guinea fowl eggshells
Fig. 3. Freundlich isotherm for the adsorption of cadmium in landfill leachate by guinea fowl eggshells
Fig. 4. Freundlich isotherm graph for the adsorption of nickel in landfill leachate by guinea fowl eggshells
CONCLUSIONS
Guinea fowl eggshells can be used for cadmium and nickel removal in landfill leachate, making this adsorbent a candidate for water remediation. The adsorption efficacies of cadmium and nickel by guinea fowl eggshells were 90.5% to 96.5% and 96.1% to 99.3%, respectively. The Langmuir isotherm suited the experimental results for cadmium and nickel. Guinea fowl eggshells can be used as a low-cost adsorbent for Ni and Cd removal from the leachate under certain conditions. Therefore, the conversion of guinea fowl eggshells in large volumes and at low-cost into green adsorbent can be applied for the adsorption of toxic metals in landfill leachate and wastewater. As a means of waste management through recycling waste and eco-friendly materials. The guinea fowl eggshell powder can adsorb higher concentrations of toxic metals from wastewater in practical application systems. Guinea fowl eggshells are readily available and inexpensive. More adsorptive research should be carried out using different eggshells as a low cost green adsorbent to remediate other toxic metals from the environment.
ACKNOWLEDGEMENT
The authors thank to Mr. Justin Kan-uge for his assistance and Mr. Prince Owusu (a Technician in the Ecological Laboratory, University of Ghana) for the samples analysis.
Conflict of Interest
Authors have no conflicts of interest.
Data Availability Statement
The original contributions presented in the study are included in the article / supplementary material, further inquiries can be directed to the corresponding author.
Author Contributions
All authors contributed equally to the conceptualisation, drafting, and editing of the research article.
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Article submitted: March 15, 2023; Peer review completed: April 15, 2023; Revised version received and accepted: May 2, 2023; Published: May 11, 2023.
DOI: 10.15376/biores.18.3.4519-4531