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Efficient Removal of Methylene Blue Dye by Alkaline-treated Banana Stem Biochar through Adsorption Method

Umesh Kumar*, Bhalchandra Vibhute, Nikhil Sharma, Abhinav Sahay

Research Scholar, School of technology, RK University, Rajkot-360020, Gujarat, India

Abstract: The design of low-cost adsorption columns for the removal of industrial effluents or other adsorption processes aids in the treatment of wastewater. The present work was intended to treat or minimise the level of contaminants in polluted water using adsorption technology. To fulfil the objectives of the study, banana stem and Alkaline-treated banana stem biochar (ATBSB) were used for the adsorption study, and these two banana tissue were used as adsorbents. Methylene blue (MB) dye was used as an adsorbate. The removal of MB dye from waste water using banana stem and ATBSB were investigated via batch mode in these studies. The given parameter were used pH 2-12, contact time 10-120 minute, adsorbent dose 0.2-2 gram, rpm 150, temperature 300k and dye concentration 25,50,75 and 100 ppm. The various adsorption isotherms like Langmuir and Freundlich were studies. In this experiment, kinetic studies include fist order, second order were carried out. The results of the adsorption study showed that the percentage removal efficiency was found to be for banana stem, 93.3 % at Ph 8, contact time 80 minute, rpm 150, temperature 300 k and 1 gram adsorbent in 50 ml MB dye solution at initial concentration 25ppm. For Alkaline-treated banana stem biochar, 96.59 % in 0.8 gram adsorbent dose with respect of constant time, pH, rpm, and temperature. The study concluded that the maximum percentage by dye removal of Alkaline-treated banana stem biochar was more efficient than that of banana stems. This work can help in designing low-cost adsorption columns for the removal of industrial effluents or other adsorption processes which help to maintain health hazards, water pollution, ecosystems and sustainable development.

Keywords: Methylene blue dyes, Adsorption isotherm, Banana stem, Alkaline-treated banana stem biochar

Received March 05, 2022; Revised April 08, 2022; Accepted April 15, 2022

Citation: Umesh Kumar, Bhalchandra Vibhute, Nikhil Sharma, Abhinav Sahay, Efficient Removal of Methylene Blue Dye by Alkaline-treated Banana Stem Biochar through Adsorption Method. Applied Ecology and Environmental Sciences, 10 (4). 236-243. January 2022. doi:10.12691/aees-10-4-8

1. Introduction

In various parts of the globe, the fresh water is a limiting resource and it will be continuously decreasing in the next decade. The continuous and regular decrease of fresh water resource is due to the increase in population density, deforestations, coal mining activities, and climate change.

[1] The increase in the population density leads to the increase in the cost of purification of water for drinking purpose because wastewater contains the pollutants like heavy metals and chlorinated organic compounds. The continuous of these heavy metals can harm human health and the entire ecosystems [2].

Industries like plastics and paper, dyestuffs, textile have used dyes as a colour their products and also consume a large amount of the water. As a result, they generate a huge amount of dye effluent in to the aquatic environment. It is recognized that public perception of water quality is greatly influenced by the colour. It is reported that colour in the water is the initial and first contaminant to be recognized in the wastewater.

The basic identification of the contaminants in the wastewater is the change in colour, and it must be removed before discharging the water into the environment [3]. Various methods have been used to minimize the pollution level in wastewater. Some of the techniques are aerobic and anaerobic microbial degradation, precipitation and coagulation, chemical oxidation, filtration and membrane separation, electrochemical treatment, and reverse osmosis. The most feasible and alternative technique for the removal of pollutant form wastewater is adsorption method [4,5].

There are several works which reported the use of adsorbents to clean the water. Some of the adsorbents are activated carbon [6,7,8], sawdust, brown coal, and bagasse [9]. These are the reported adsorbents which are used to remove colour from wastewater [10]

Through various literature surveys, it is revealed that certain biological materials like rice husk, orange peels, tea leaves and wheat straw have also been used as adsorbents to remove dye from wastewater.

The removal of dye from wastewater during agricultural biomass-based adsorbents has newly concerned the interest of the scientific community owing to good removal capacity with least amount environmental crash. On the other hand, most agricultural bio-adsorbent undergo from immovability issues and frequently discharge soluble components into water during the adsorption process. Methylene blue (MB) is a heterocyclic aromatic compound used as a medication or as a synthetic dye for textiles. Due to its ecotoxicity, researchers have been investigating its mitigation by the adsorption process.

Over the last twenty years, the production and environmental applications of biochar have gained considerable attention. This emerging eco-economical carbonaceous product is produced via simple slow or fast pyrolysis of precursor biomass without any activation. The global abundance of raw materials and its one-step production process makes it a cost-effective and sustainable material. The final properties of biochar mainly depend on the physicochemical properties of biomass and its processing conditions like temperature, heating time, and heating rate. Therefore, these physicochemical properties can be controlled by selecting a proper precursor and altering process condition to achieve maximum efficiency to specific applications.

2. Materials and Methods

In the present study, the Methylene blue (MB) dye was used, and the dye was a product of German Merck Company. The MB is a heterocyclic aromatic chemical compound with the molecular formula C₁₆H₁₈N₃SCl [Figure 1]. It is used as a stain and also as a pharmaceutical drug. It is a solid and dark green powder at room temperature. When it is dissolved in water then it shows as a blue solution. The exposure of MB dye can cause eye burns which in turn results in the permanent injury to the eyes. The inhalation of MB dye can cause breathing problem, nausea, vomiting, and mental confusion. Hence the removal of MB dye from the industrial effluent has become a great concern for the researchers.

For this purpose, the low-cost adsorbents namely Banana stem was selected. The specific plant was selected due to the easily available of the plant species. Banana stems were taken from local market of Rajkot, Gujarat The adsorbate used in this study was Methylene blue dye (Merck) of powder, which was purchased from Merck science private Limited, Mumbai.

Figure 1. Chemical structure of methylene blue

A calibration curve of optical densities against methylene blue concentrations was obtained by using standard methylene blue solution at natural pH. calibration cure shows the beer’s law is obeyed in concentration range [0-12mg/l] the experimental data show in Figure 2 were fitted by a straight line with correlation coefficient (R2 = 0.994).

Figure 2. Standard curve of Methylene blue dye

2.1. Preparation of Banana Stem as Adsorbent

Banana stems were used as low cost adsorbent. (Figure 3) The banana stems were collected and cut them into small pieces separately. They were washed with distilled water to remove dust particles and keep them into water for 2-3 minutes. Banana stem was dried into hot air oven at 120°C for 24 hours. Dried stem was powered by domestic mixture. It was sieved at 150 µm thus powder of banana stem adsorbent is prepared. It is a natural adsorbent, without use any chemical for preparation of powder form.

Figure 3. Banana stem

2.2. Preparation of Alkaline-treated Banana Stem Biochar (ATBSB)

100-gram measured amount of dried banana stem sample was kept in an enclosed crucible covered with aluminum foil and afterward heated at ideal temperatures by slow pyrolysis in an electrical muffle furnace [11]. After completion of the pyrolysis process, the remaining biochar was allowed to cool to room temperature. It was showed in Figure 4. Further, it was immersed in 1 M NaOH solution for 1 hour which increases in the number of active surfaces of Banana stem biochar. [12] It was responsible for the prevention of the elution of tannin compounds. [13]. The sample was frequently washed with distilled water for the removal of NaOH solution. Sample was dried at 105 °C for 48 hours. The dried sample was crushed and passed through a range of sieves with 425 microns [14]. Further, the sample was dried for 2 hours in an oven at 80–85°C. The processed samples were stored in airtight bags until use.

Figure 4. Alkaline-treated banana stems

2.3. Adsorption Capacity and Removal Efficiency of Methylene Blue

The amount of Methylene blue adsorbed per unit adsorbent was calculated according to a mass balance on the Methylene blue concentration using the following Equation (1).

[picture] | (1)

Where Ci is the initial Methylene blue concentration (mgL⁻¹), Cf is the equilibrium Methylene blue concentration in solution (mgL⁻¹), V is the volume of the solution (L) and m is the mass of the adsorbent in gram.

The (%) adsorption of Methylene blue was calculated using the given equation (2)

[picture] | (2)

Where Co is the initial Methylene blue concentration (mgL⁻¹), Cf is the equilibrium Methylene blue concentration in solution (mgL⁻¹).

2.4. Batch Adsorption Studies

The batch adsorption experiments were conducted in laboratory to study optimum removal of methylene blue dye from aqueous solution. The experiment regarding the adsorption of MB on to the ATBSB and Banana stem surface were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with different adsorbent dosages. Then the samples were kept in orbit shaker at 30⁰c temperature at 150 rpm at constant time and pH. Afterward the samples were filtered using whatman paper no 42 to separate the adsorbents from MB Solution. Finally, the residual concentration of MB were measured using UV-visible spectrophotometer (SL 159, ELICO, connecting science & lab) at its maximum absorbance wavelength 663nm. The same experiment had done at different condition to find out the equilibrium time, optimum doge of adsorbent and pH.

2.4.1. Adsorption Isotherm

Adsorption isotherms have been of immense importance to researches dealing with environmental protection and adsorption techniques. The two primary methods used for predicting the adsorption capacity of a given material are known as the Freundlich and Langmuir isotherms. [15]

3. Results and Discussion

3.1. Adsorbent Properties

The adsorbent were categorized by FTIR in a close by IR region (wave number: 400–4,000 cm⁻¹). The FTIR spectra were displayed absorption peaks related to diverse functional groups. The wave number of 3,500 cm⁻¹ shows the hydroxyl (–OH) stretching, even as the wave number of 3000 cm⁻¹ are recognized to the aliphatic C–H stretching.

Figure 5. FTIR spectra of banana stem Raw

Figure 6. FTIR spectra of ATBSB

The band at around 1100 cm⁻¹, which shows a peak very strong, it may happened due to some shaking of inorganic ingredients. An assessment between the FTIR spectra of the banana stem raw (Figure 5) and of ATBSB (Figure 6) were changed in absorption frequencies at 3,000, and 3,500 cm⁻¹, due to presented in the surface of the adsorbent. It proves that the mentioned functional groups influence the MB adsorption on the banana stem in experiment.

3.2. Batch adsorption Studies of Banana Stem

3.2.1. Effect of Contact Time

Contact time was evaluated as an important factor affecting adsorption efficiency. It was reported that the percentage of removal increased with increased contact time [16].

The percentage removal of methylene blue was increased as the agitation time is increased from 10-120 minute. Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with 500 mg adsorbent dosages of banana stem. Then the samples were kept in orbit shaker at 30⁰c temperature at 150 rpm at constant rate. The maximum percentage removal of methylene blue dye is obtained 85.82% at 80 minutes. with 25 ppm. The increasing the agitation time from 10-120 minute the % removal of MB dye is also increasing (Figure 7).

Figure 7. Effect of contact time on MB adsorption

3.2.2. Effect of Banana Stem Adsorbent Dose

Figure 8 shows the removal of MB dye by banana stem at different dose of adsorbent (0.2 – 2 g). Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution. Then the samples were kept in orbit shaker at 30°C temperature at 150 rpm at 80 minutes. The maximum percentage removal of methylene blue dye is obtained 93.3 % at 1 g dosage of adsorbent. (Figure 8)

Figure 8. Effect of adsorbent dose on MB adsorption

3.2.3. Effect of the pH

The pH of the dye solution is very important factor for adsorption of dye on the adsorbent. This is due to the variation of pH leads to the variation of degree of ionization of the dye molecule and surface properties of the adsorbent [17]. Dye removal was studied at pH ranging between 2 and 12 by maintaining pH of sample with dilute 0.1 N HCl or 0.1 N NaOH solutions. Normally, the percentage of dye removal would be decline for cationic dye adsorption at the low pH solution, whereas the percentage of dye removal will increase for anionic dyes. In contrast, the percentage of dye removal will increase for cationic dye adsorption at a high pH solution and decrease for anionic dye adsorption. [18]

The percentage removal of methylene blue was increased the different pH 2-12. Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with 1g adsorbent dosages of banana stem. Then the samples were kept in orbit shaker at 30°C temperature at 150 rpm at 80 minutes. The maximum percentage removal of methylene blue dye is obtained 96.6% at pH 8. (Figure 9)

Figure 9. Effect of pH on MB adsorption

3.3. Batch Adsorption Studies of ATBSB

3.3.1. Effect of ATBSB Adsorbent Dosage

Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with different ATBSB adsorbent dosage (0.2 – 2 g). Then the samples were kept in orbit shaker at 30°C temperature at 150 rpm at 80 minutes. The maximum percentage removal of methylene blue dye is obtained 96.59 % at 0.8 g dosage of adsorbent. (Figure 10)

Figure 10. Effect of ATBSB adsorbent dosage on MB adsorption

3.3.2. Effect of Contact Time

The percentage removal of methylene blue was increased as the agitation time is increased from 10-120 minute. Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with 0.8 gram adsorbent dosages of ATBSB. Then the samples were kept in orbit shaker at 30°C temperature at 150 rpm at constant rate. The maximum percentage removal of methylene blue dye is obtained 97.50 % at 50 minutes with 25 ppm. (Figure 11)

Figure 11. Effect of Time on MB adsorption

3.3.3. Effect of the Ph

The percentage removal of Methylene blue was increased the different pH 2-12. Experiments were conducted in 100ml Erlenmeyer flasks containing 50mL of MB solution in different ppm (25, 50, 75 and 100) dye solution with 0.8 gram adsorbent dosages of ATBSB. Then the samples were kept in orbit shaker at 30⁰c temperature at 150 rpm at 50 minutes. The maximum percentage removal of Methylene blue dye is obtained 98.6% at pH 8. Graph shows in Figure 12.

Figure 12. Effect of pH on MB adsorption

3.4. Adsorption Characteristic of Banana Stem and Alkaline-treated Banana Stem Biochar

The adsorption isotherms have exposed the unique relation between the concentration of adsorbate and its adsorption quantity onto adsorbent surface at a constant pH and temperature. The Langmuir isotherm, Freundlich isotherm and Temkin isotherm were used to specify the adsorption capacity of Banana stem and Alkaline-treated banana stem biochar for the removal of MB dye from aqueous solution.

3.4.1. Langmuir Isotherm

This model assumes that the adsorption occurs at definite homogeneous site on the adsorbent. It is used effectively in various monolayer adsorption processes [19]. This isotherm is appropriate for monolayer adsorption on the surface having an inadequate number of the same sites. It describes the structure of a monolayer adsorbate on the surface of the adsorbent.

The equation of Langmuir is given equation 3:

[picture] | (3)

Where, qe (mgg⁻¹) is the adsorption capacity, Ce is the concentration of dye solution (mg/L⁻¹), kL is related to the affinity of the binding sites, qm (mgg⁻¹) is signifies the maximum monolayer adsorption capacity whish depends on the number of adsorptions.

An additional analysis of the Langmuir isotherm can be made in terms of dimensionless equilibrium parameter RL in equation 4

[picture] | (4)

The value of RL lies between 0 and 1 for the favourable adsorption, even as RL > 1 shows the unfavourable adsorption and for linear adsorption RL=1. If RL =0 Then it represent irreversible adsorption.

Figure 13. Langmuir isotherm for adsorption of Methylene Blue onto banana stem powder at pH 8, contact time 80 minute , and adsorbent dose 0.2g – 2g

Figure 14. Langmuir isotherm for adsorption of Methylene Blue onto Alkaline-treated banana stem biochar at pH 8, contact time 50 minute, and adsorbent dose 0.2g – 2g.

Table 1. Langmuir Isotherm constants for adsorption of methylene blue onto banana stem and Alkaline-treated banana stem biochar

Based on the Figure 13 and Figure 14, the Langmuir isotherm parameters were calculated in Table 1. Here the value of R2 for MB dye adsorption was 0.998 and 0.999. It suggested that the adsorption Langmuir model and the values of RL for both the adsorbent lies between 0 and 1 indicating favourable adsorption of the dye onto the adsorbents [20]. The value of RL was 0.99928 which indicates favorable adsorption.

3.4.2. Freundlich Isotherm

The Freundlich isotherm can be functional for non-ideal sorption on heterogeneous surface and multilayer sorption. The equation of Freundlich is given in equation 5

[picture] | (5)

Where, KF is Freundlich equilibrium constant, n is equilibrium constant.

Figure 15. Freundlich Isotherm for adsorption of Methylene Blue onto banana stem powder at pH 8, contact time 80 minute , and adsorbent dose 0.2g – 2g

Figure 16. Freundlich Isotherm for adsorption of Methylene Blue onto Alkaline-treated banana stem biochar at pH 8, contact time 50 minutes, and adsorbent dose 0.2g – 2g

Table 2. Freundlich Isotherm constants for adsorption of methylene blue onto banana stem and Alkaline-treated banana stem biochar

Based on the Figure 15 and Figure 16, the Freundlich Isotherm parameters were calculated in Table 2. Here the value of R2 for MB dye adsorption was 0.864 and 0.811. It suggested that the adsorption Freundlich Isotherm model and the values of n satisfy the condition 1< n <10 then it was considered as favourable otherwise unfavourable. While the n values for adsorption of MB in both the cases more than 10 therefore it is indicating unfavourable adsorption process. The value of KF was 0.42954 and 0.50933 which indicates favorable adsorption. The experimental data fitted well with Freundlich isotherm, but the value of n was 22.72 and 13.33 which did not satisfy the condition 1< n <10. Then it is indicating unfavourable adsorption process.

3.4.3. Temkin Isotherm

The Temkin isotherm model assumes that the adsorption heat of all molecules decreases linearly with the increase in coverage of the adsorbent surface. The Temkin isotherm is given in equation 6

[picture] | (6)

Figure 17. Temkin Isotherm for adsorption of Methylene Blue onto banana stem

Figure 18. Temkin Isotherm for adsorption of Methylene Blue onto Alkaline-treated banana stem biochar

Table 3. Temkin Isotherm constants for adsorption of Methylene blue onto banana stem and Alkaline-treated banana stem biochar

Based on the Figure 17 and Figure 18, the Temkin Isotherm parameters were calculated in Table 3. In this graph BT has a positive value that means adsorption process is exothermic. The value of BT is 0.028. The value of AT, describe the affinity of the sorbent for adsorbent. Here the value of R2 for MB dye adsorption was 0.859 and 0.814. It indicated that the Temkin isotherm achieved a good fit for the adsorption data with R2 > 0.99 and strong interaction between the MB and the reactive group.

4. Conclusions

The work concluded that the adsorbents which were used in this study can be used in the designing of low-cost adsorption columns for the removal of industrial effluent or other adsorption processes. By varying different parameters like pH, contact time, and adsorbent dosage the maximum percentage removal of the pollutant in the wastewater can be achieved by using batch adsorption process in natural treatment. The present work is a novel work, which can be used for the treatment of large amount of MB Dye wastewater through adsorption technology. We have got result after experiment maximum 93.3 % MB dye removal at Ph 8, contact time 80 minutes, rpm 150, temperature 300 k and 1 gram adsorbent in 50 ml MB dye solution at initial concentration 25ppm by using batch adsorption process in banana stem as well as 96.59 % MB dye removal from 0.8 gram adsorbent dose with respect of constant time, pH, rpm, and temperature by alkaline-treated banana stem biochar. Equilibrium data fixed very well in the Langmuir isotherm equation, conforming the monolayer adsorption capacity of MB onto banana stem and alkaline-treated banana stem biochar. A linear plot was drawn for Langmuir and Freundlich isotherm in both the adsorbent. In the Langmuir isotherm, the value of RL lies between 0 and 1 indicating favourable adsorption While the n values for adsorption of MB in the freundlich isotherm more than 10 therefore it is indicating unfavorable adsorption process. Temkin Isotherm parameters were calculated, and BT has a positive value that means adsorption process is exothermic. Adsorption Isotherm concluded that the adsorption of MB on the banana stem and alkaline-treated banana stem biochar adsorbent followed Langmuir model with the monolayer phenomena in exothermic condition.

Lastly the adsorption experiments indicate that alkaline-treated banana stem biochar has very good adsorption capacity for basic dye in aqueous solution compared to banana stem adsorbent without chemical treatment. Banana stem, an agricultural waste material can be effectively used for the preparation of biochar. The lab scale data can be used as baseline data for designing treatment plants for removal of MB dye containing effluents

Acknowledgments

The first author (Umesh Kumar) is highly indebted to Environmental Engineering Department, School of Engineering, Faculty of Technology, RK University, Rajkot, for providing platforms like research laboratories, chemicals, etc., to do this research work. I also thank Mr. Nikhil Sharma and Abhinav Sahay (Co-author) for editing this paper.

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