Environmental engineering studies aim is to use lowcost materials mostly from natural wastes as a Sorbent. Removing heavy metals from simulated wastewater solutions using chemically modified orange peel named (MOP) was examined at various pH, adsorbent doses, and temperature on the single heavy metal solution. Experiments of the batch were executed according to optimal conditions to estimate the sorption ability MOP. The results present ahighcapacity of the sorption by MOP of about 91.0 % and 93.44% for Cd (II) and Ni (II) Consecutively,with the optimum amount of sorbent of MOP about 3gm and 2.5gm at pH 6; with contact time 180min at 298K temperature. It was found that the efficiency of sorption of MOP decreased by increasing the temperature showed the sorptionnature is exothermic. The mass transfer adequacy in the adsorption process using thesesustainable low cost modified orange peels make it efficient in removing heavy metals. The study ofequilibrium isotherm and kinetic models of both ions sorption by adsorbents were evaluated, the isotherm of Langmuir was assessedto be the suitable equation for Cd (II) ion removal. In contrast, the suitable model for Ni (II) removal was Freundlich, and a 2nd kinetic model was utilized to estimate the kinetic constants of the overall rate of sorption for both ions. MOP showsa high impact in removing ions of cadmium and nickel from an aqueous solution.
See discussions, stats, and author profiles for this publication at: https://www.researchgate.net/publication/347973940 Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution Article in Journal of Green Engineering · November 2020 CITATION READS 162 authors: Lahieb Faisal Muhaisen Shahad Al-Najjar Independent Researcher Al-Nahrain University 10 PUBLICATIONS 45 CITATIONS 11 PUBLICATIONS 16 CITATIONS SEE PROFILE Zainab T Al-sharify Al-Mustansiriya University 171 PUBLICATIONS 131 CITATIONS SEE PROFILE Some of the authors of this publication are also working on these related projects: sustainability View project Using Positron Emission tomography (PET) scan for tumar detection View project All content following this page was uploaded by Lahieb Faisal Muhaisen on 29 December 2020 The user has requested enhancement of the downloaded file SEE PROFILE Journal of Green Engineering (JGE) Volume-10, Issue-11, November 2020 Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution M Lahieb Faisal, 2Shahad Z Al-Najjar, 3Zainab T Al-Sharify Department of Environmental Engineering, College of Engineering, University of Mustansirya, Baghdad, Iraq Department of Chemical Engineering, College of Engineering, Al-Nahrain University, Baghdad, Iraq School of Chemical Engineering, University of Birmingham, Birmingham, United Kingdom E-mail: z.t.alsharify@uomustansiriyah.edu.iq, zta011@alumni.bham.ac.uk Abstract Environmental engineering studies aim is to use low-cost materials mostly from natural wastes as a Sorbent Removing heavy metals from simulated wastewater solutions using chemically modified orange peel named (MOP) was examined at various pH, adsorbent doses, and temperature on the single heavy metal solution Experiments of the batch were executed according to optimal conditions to estimate the sorption ability MOP The results present ahighcapacity of the sorption by MOP of about 91.0 % and 93.44% for Cd (II) and Ni (II) Consecutively,with the optimum amount of sorbent of MOP about 3gm and 2.5gm at pH 6; with contact time 180min at 298K temperature It was found that the efficiency of sorption of MOP decreased by increasing the temperature showed the sorption-nature is exothermic The mass transfer adequacy in the adsorption process using thesesustainable low cost modified orange peels make it efficient in removing heavy metals The study ofequilibrium isotherm and kinetic models of both ions sorption by adsorbents were evaluated, the isotherm of Langmuir was assessedto be the suitable equation for Cd (II) ion removal In contrast, the suitable model for Ni (II) removal was Freundlich, and a 2nd kinetic model was utilized to estimate the kinetic constants of the overall rate of sorption for both Journal of Green Engineering, Vol 10_11, 10600-10615 © 2020 Alpha Publishers All rights reserved 10601 M Lahieb Faisal et al ions MOP showsa high impact in removing ions of cadmium and nickel from an aqueous solution Keywords: Wastewater, Heavy Metals, Fluid Flow, Environmental Engineering Studies, Cd (II), Ni (II), Mass Transfer, Modified Orange Peel (MOP), Exothermic Introduction Heavy metals is crucial pollutants in the water sources and industrial water-treatment Hence,a severepublic health issue is developing every day byaccumulating the heavy metals'existence Electroplating, finishing of metal, and metallurgical are some examples of the leadingcauses of these heavy metals and the chemical manufacturing, mining, and processes of battery manufacturing in large quantities Heavy metals are recognized as toxic components, and their deposals throughstreams are causingunfavorable effects on the health of humans alike the environment [1][2][3] Compoundsof the toxic metal pollute the sources of surface water andother sources as well [4] [5] They cause many health disorders and disturbances Also, because of their toxicity, the existence of metals in unreasonable amounts intervenes with the profitable utilize of water [1] [2] [3] It is also essential to find a way to get rid of metals in wastewater before dumped into the atmosphere Nickel is a pure white alloy, has a radioactive amount of 28 Drinking water, normally contains Ni of less than ten mg/l, where the typical day-by-day intake of Ni from water for adults maybe around 7.5 and 15 mg [6][7][8] Ni and its components are returned to outstanding hazardous specialists encountered by additionally proven non-occupationally uncovered people in the industry [5][7].Cadmium hasa lot of observation by ecologists as one of the most toxic heavy metals [9] [10] [4] [11][12] High-quality water is necessary to a human's life; water with reasonable quality is vital for domestic, agricultural, commercial, and industrial uses [13] Many researchers recently investigate experimentally and numerically using CFD of the fluid flow of single-phase flow contaminates and multi-phase flow contaminates [14-19] From all the above, it was observed that all these activities are responsible for water pollution Every day vast quantities of waste are dumped from these sources into freshwater The need for water is increasing as all water resources slowly become unusable because of inappropriate disposal of waste [20] The mission of providing suitable treatment facilitiesfor all sources of contaminationis challenging and costly, so there is an urgent need for innovative, low-cost technologies that require low maintenance and energy-efficient The use of different techniques is mostly sufficient to remove heavy metals from water and wastewater [21, 22,23]; from these, sorption is efficient and economical Considered sorption onto activated carbon is a preferredmethod that has been widely utilized in Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution 10602 the past few years Because The need to achieve economical treatment of wastewater iscrucial, the researchers intensified their efforts to finding and developing inexpensive alternatives available from various industrial, natural, and biological materials or residues [20] The majority of researchers used numerous of fruit peel as a substitution of activated carbon due to its high-priced The use of agricultural-residues as the sorbent is attracting attention on a large scale because of the availability of large amounts [24, 25] Also, a polysaccharide of the top plants' cell wall, Pectin, is predominantly depending on the acid of galacturonic and contains a considerable number of groups of carboxyl, with a familiar capability to contain bi-valence cations Thus, a material rich in Pectin, like citrus peels resulting from the Pectin is removed commercially, has a high natural capability to bind the metal The Pectin-rich products have been considered in the potential to bind metal to involve: waste of apple; sugar beet pulp; peels of orange and banana; citrus peels and husksof coffee, alsomany kindsof fruit, like various kinds of citrus peel [26-31] Besides, Natural Sorbent such as Rice Husk [32], dried olive stone [33], most recently walnuts Shell as an adsorbent from wastewater contaminated with COVID 19 viruses [34] Orange peel is is normally treated as wastes, although it have a lot of functional groups, as hydroxyl and carboxyl make it a potential sorbent material inthe removal of metals [35] Some researchers suggested in the literature the ability to utilize the modified waste of orange in rapport with adsorptionof heavy metal from water [36,37,38] This work aimed to provide anadsorbent of modified orange peel (MOP) and assess this sorbent's sorbent ability in removing two heavy metal ions (Cd2+ and Ni2+) Experimental 2.1 Chemicals The synthetic solution of cadmium ion and nickel ion provided by dissolving the Cd (NO3)2.4H2O and N2NiO6.6H2O with distilled water; to prepare the desired initial concentration was according to Eq.1 [39]: (1) Where: Wt is the heavy metal salt-weight, mg; V is the volume of the solution, 1liter Cp is theprimary concentration of metal ions in solution, mg/l; M.wt is themetal salt molecular weight, g/mole; At.wt is the metal ion atomic weight of, g/mole 10603 M Lahieb Faisal et al To adjust the solution's pH to the wanted amount, (0.1M) HCl or (0.1M) NaOH as needed has been added Atomic Absorption spectrophotometer has been used to estimate cadmium and nickel (AAS, GBC 933 plus, Australia) 2.2 Preparation of Modified Orange Peel Adsorbent Generally, the peels of chemically modified agricultural waste show an increasingbiosorption capacity than the non-modified types Several chemicals have beentested to containorganic acids and minerals, oxidizing agents, bases, and organic components In the natural state the agriculturalpeel or husk has a high content of lignin, hemicelluloses, cellulose, and mineral ash [40] The charge ofthissurface of cellulosic will be partially negativewhen submerging in water, thus producinga Colombian reaction with the species of cationic in water, Laszlo and Baig [41] checked on the binding of Cr+2, Ni+2, Pb+2, Cu+2,Zn+2, Cd+2and Cr+2ions to the deactivated biomass of Solanum Elaeagnifoliumand proposed that the collectionsofcarboxyl (—COOH) are somewhat in charge of the binding of ions of metal [42] Orange Peel (OP) in this paper was gathered from the local market of juice andwashed with distilled water many times for removingthe dirt; dried at 100oC for 24 hours in the oven (until steady weight)dueto removing the content of moisture.This dried peel grinded and sieved to get about 0.6 mm size of the particles were chosen for this study Then 10 gm of dried OPsaturated by a50mL solution ofNaOH (0.1 M) for 6hrs (this intensifiedpeel treated with sodium hydroxide to enhance sorption capacities to proposed ions); then using filtration The orange peel (MOP) changed in sodium hydroxide had been washed with purified water up to 7.0 pH value; then washed and placed in airtight vessels for use 2.3 Adsorption Procedure and Measurement All adsorption tests were carried out on the batch type.Wastewater solution of desired concentration (50mg/l) (for each ions) was taken with the required amount of MOP (1-3.5gm) in 250ml Erlenmeyer flasksto examine the impact of treated sorbent on the removal of Cd+2and Ni+2a 100ml and then shaken with fixedagitation speed (200 rpm) at a room temperature (approximately 25±5°C) for a contact time of 180min The pH was adjusted to (3-8) The supernatant was separated by filtration (using filter-paper Whatman70mm) Initial and final concen.of both ions were specified by the (AAS) The equation (2) used todetermine the amount of both ions sorbed by the MOP was as follows [39]: (2) Where Cfis thefinal concentration of the metal, mg/l Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution 10604 Results and Discussion 3.1 Impact of PH on the Sorption Process As is customary, thepH is a determining parameterthat governs the sorption of the metal ions These ions influence protonsof the functional groups as well as in the chemistry of metal [43] Figure1 presents the removal of Cd+2 and Ni+2 at varying pH ranges from to (with g of the MOP sorbents used for contact time about 1hr) It evidentfrom the results (Fig.1a and b) that the removal of studied ions increased significantly with high pH values The higher rate of sorption of both ions was noticed at pH range between to 6, and the efficiency gradually decreasesby increasing pH values 9(At low values ofpH, metal cations and protons contest for sites of binding on the surface of sorbent, which contributes to decrease themetal uptake It was indicated that the sorbent surface ligands in a quite acidic state were closely bound to H3O+, which, due to repulsive forces, restricted access to ligands by metal ions [8, 26 , 44].As pH values rise, it is anticipated that more ligands would be exposed to negative loads, leading to an improvement in the appeal of positively charged metal ions The weaker association is often due to the metal's lower solubility and precipitation [8, 44-51] while pH is greater For Cd+2 and Ni+2 ions, the maximum removal at pH is then acquired with a sequential efficiency of 82 percent and 86 percent Figure Impact of PH on the Sorption Process (a: Cd (II); b: Ni (II)) 10605 M Lahieb Faisal et al 3.2 Impact of MOP Amount on the Sorption Process The influence of MOP sorbents amounts to one of the generally influential parameters affecting the capacity of removal and the capacityofsorption Figure shows the impact of various quantities of sorbents (1-3.5 g/100ml) for hours at room temperature The sorption efficiency of Cd2+ and Ni2+ increased with increasing the concentrations of metal ions and quantityof MOP;this behavior is mainly due to the increase in the surface area of sportive and the availability of more effectivesites of sorption [19, 29].The maximum removal of Cd+2has been made at more than 2gm of MOP sorbent The optimum amount was chosen as 3gm with the removal rate of about 91%, while removing Ni+2was at 2.5gm of MOP sorbent with the removal of about 91.11%.After more increase in sorbent weights than 3gm we notice that no effect on the removal rate because the adsorbent was sufficient to adsorb [44, 45] Figure Impact of MOP Amount on the Sorption Process (a: Cd (II); b: Ni (II)) 3.3 Sorption Isotherm The modeled adsorption isotherm is calculated utilizing two known isothermal models i.e., Freundlich and Langmuir, for single soluble Systems Adsorption isotherm should be used by characterizing how the solution reacts with the adsorbent to boost adsorbent use [45].The Langmuir sorption Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution 10606 isotherm equation, showed as follows, requires for its applicability singlelayer coverage on the adsorbent surface[39]: ( ) (3) Where: is the biomass sorbed metal ions, mg per each gram, is the ability of the highest of sorption for monolayer coverage, mg per each gram, b is the attraction site constant of binding, mg per liter is the metal ions concentration in the solution at balance, mg per liter The model of Freundlich is [24]: (Linear form) (4) K = constant refer the relativecapability of adsorption of the adsorbent (mg/g), 1/n = constant expressing the adsorption potential K and n presented a range of adsorption See Fig.3 (A and B) and Table 1, which shows the above two models' results Figure 3(A) Langmuir Model (a: Cd (II); b: Ni (II)) 10607 M Lahieb Faisal et al Figure (3B) Freundlich Model (a: Cd (II); b: Ni (II)) Table The Parameters of Isotherm Models Langmuir coefficients R2 A B Cd (II) Ni (II) 0.9767 3.3602 0.1794 0.8672 5.7310 0.1895 Freundlich coefficients R2 N K Cd (II) Ni (II) 0.8683 2.3912 0.7951 0.9336 1.7819 0.7995 Compared to experiential isotherms, the equation Langmuir was ideal for eliminating Cd (II) ions with the theoretical isotherm models.In contrast, the Freundlich model is more adequate to remove Ni (II) ions by using MOP as sorbents 3.4 Kinetic Isotherm The mechanization of dye sorption is described by the kinetics of adsorption (pseudo-first and second-order).Models describethe adsorption manner of both ions on MOP The pseudo-first and-second-order models, [39]: (5) ( ) Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution 10608 ( ) (6) The sum of dye adsorbed in balance and qeq(mg/g) and qt (mg/g) in a corresponding period For the pseudo-first and second-order models, K1 (min−1) and K2 (g/mg.min) are equal to a constant kinetic volume The findings were shown in Table Table The Factors of Kinetic Models Metal T aCd b(II) l eNi (II) Pseudo-first-order qeexperimental Pseudo-second-order qecalculate k2 R2 k1 1/min qecalculated R 1.530 -0.0385 1.0710 0.9203 0.1155 1.580 0.9976 1.956 -0.0386 1.5221 0.8108 0.0998 1.9992 0.9982 d Table has shown that qe (theoretical)'s results are well-accepted in the case of the pseudo-second-order constructs with the experiential uptake measures qe(exp) The correlation(R2) factor was 0.9976 and 0.9982, respectively for Cd(II) and Ni(II) suggesting that the pseudo-sections phase for both ions may also be represented 3.5 Impact of Temperature and Thermodynamic Parameters It is well established that thermodynamic studies will determine the physical and chemical adsorption response direction and viability "These thermodynamic parameters are normal enthalpy (alternative to H°), standard free energy (alternative to G°), standard entropy (Alternative to S°)' From the following equation, the values of these parameters were obtained [9, 24]: ( ) ( ) (7) (8) ΔG=ΔH-ΔST In which Kd the distribution coefficient; while ΔH, ΔS,and ΔT the enthalpy, entropy, and temperatures R is the gas constants (8,314 J/mol.K) and Gibbs free energy change ΔG0 Impact of changing the temperature at 298, 308, 318, and 328K (25, 35,45 and 55Co) "Fig.4", the coefficient values of distribution and the parameters of thermodynamic arescheduledin Tables and 4, consecutively: 10609 M Lahieb Faisal et al Figure Impact of various temperatures on sorption of both ions by MOP (a: Cd (II); b: Ni (II)) Table The Coefficients Ofdistribution At Various Temperatures Metal Cd (II) Ni (II) R2 kd 298 k 308 k 318 k 328 k 9.438413 13.53488 4.760369 4.181347 3.205214 2.723008 2.132832 1.797985 0.9867 0.9380 Table The Thermal Factors of Cadmium and Nickel Ions Sorption on the MOP Metal Cd (II) Ni (II) ∆H(J/mol) ∆G (kJ/mol) 298 k 308 k 318 k 328 k -39.5954 ∆S (J/mol K) 114.7581 -284.322 -293.863 -303.404 -53.0633 158.0575 -391.599 -404.74 -417.881 312.945 431.021 Removal of both ions decreased by increasing the process temperature from 298 to 328 K at pH 6.0 for both Cd and Ni ions, respectively, and at a Modified Orange Peel as Sorbent in Removing of Heavy Metals from Aqueous Solution 10610 constant adsorption dose of 3gm and 2.5gm The decrease inthe adsorption patternby increasing the temperature valuesdetected that the qualityof sorption of Cd (II) and Ni (II) ions on MOP is exothermic Furthermore, lower values of adsorption distribution parameters (Kd) by increasing temperature also detect this process's exothermic nature The increasingcause to escapethese ions at high temperature could be other caption to this results; similar results were reported by others [44-46] Conclusions It was found that orange peel has been modified chemically by sodium hydroxide improved the removal ofCd (II) and Ni (II) ions from aqueous solution Experiential studies suggestedthat the quick removal of both ions depends mainly on the solution pH; amount of sorbent, andcontact time Negative values of (∆G) suggest the thermodynamically practical and unpromptednatureof Cd (II) and Ni (II) biosorption byMOP Thus, this studyprogressesan inexpensive, widely available,and active metalions sorbents from natural waste as a substitute for present commercial sorbents Acknowledgment The authors would like to thank Mustansiriyah University 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19, no 5, pp 1365-1370 , 2009 [45].Gonen, F., S Serin ―Adsorption study on orange peel: Removal of Ni (II) ions from aqueous solution‖, African Journal of Biotechnology, Vol 11, no 5, pp 1250-1258, 2012 [46].Arbind K., Vipin K., ―Equilibrium and thermodynamic studies of Cd (II) biosorption by chemically modified orange peel‖, Journal of Environmental Biology Vol 37, no 2, pp 201-206, 2016 Biographies Lahieb Faisal M.A is a lecturer at the Environmental Engineering Department, college of Engineering, University of Mustansiriyah She received her BSc from al Mustansiriyah university, college of Engineering and MSc from Baghdad university, college of Engineering Her research focuses on Environmental pollution 10615 M Lahieb Faisal et al Shahad Z A Al-Najjar is a lecturer at the Chemical Engineering Department, Al-Nahrain University She received her BSc and MSc from AlNahrian University, Iraq, and PhD degree form the University of Birmingham, UK Her research focuses Mass Transfer, Fluid flow, Nano particles, computational fluid dynamics and formulation technology Zainab T Al-Sharify is a lecturer of chemical engineering at the Environmental Engineering Department, University of Mustansiriyah And she is academic vistior at chemical engineering department, University of Birmingham, UK.She received her BSc and MSc from Al-Nahrian University, Iraq, and PhD degree form the University of Birmingham, UK She published more than 56 papers in peer reviewed journals Her research focuses on Fluid flow, Nano particles, computational fluid dynamics and formulation technology View publication stats