Environ Monit Assess (2014) 186:7987–7998 DOI 10.1007/s10661-014-3981-5

Nickel(II) biosorption from aqueous solutions by shrimp head biomass Alejandro Hernández-Estévez & Eliseo Cristiani-Urbina

Received: 1 December 2013 / Accepted: 25 July 2014 / Published online: 17 August 2014 # Springer International Publishing Switzerland 2014

Abstract The present study evaluates the capacity of shrimp (Farfantepenaeus aztecus) head to remove toxic Ni(II) ions from aqueous solutions. Relevant parameters that could affect the biosorption process, such as shrimp head pretreatment, solution pH level, contact time and initial Ni(II) concentration, were studied in batch systems. An increase in Ni(II) biosorption capacity and a reduction in the time required to reach Ni(II) biosorption equilibrium was manifested by shrimp head biomass pretreated by boiling in 0.5 N NaOH for 15 min; this biomass was thereafter denominated APSH. The optimum biosorption level of Ni(II) ions onto APSH was observed at pH 7.0. Biosorption increased significantly with rising initial Ni(II) concentration. In terms of biosorption dynamics, the pseudo-second-order kinetic model described Ni(II) biosorption onto APSH best. The equilibrium data adequately fitted the Langmuir isotherm model within the studied Ni(II) ion concentration range. According to this isotherm model, the maximum Ni(II) biosorption capacity of APSH was 104.22 mg/g. Results indicate that APSH could be used as a low-cost, environmentally friendly, and promising biosorbent with high biosorption capacity to remove Ni(II) from aqueous solutions.

A. Hernández-Estévez : E. Cristiani-Urbina (*) Departamento de Ingeniería Bioquímica, Escuela Nacional de Ciencias Biológicas, Instituto Politécnico Nacional, Prolongación de Carpio y Plan de Ayala s/n. Colonia Santo Tomás, México, DF 11340, Mexico e-mail: [email protected]

Keywords Biosorption . Farfantepenaeus aztecus . Nickel . Shrimp head

Introduction The discharge of heavy metal-polluted effluents from industrial and technological processes into natural water streams has turned into an expanding global problem (Gialamouidis et al. 2009; Shroff and Vaidya 2011a). Heavy metals pose severe threats to aquatic and terrestrial environments, public health, and human well-being because they are toxic, environmentally persistent, nonbiodegradable, and have a tendency to accumulate within living organisms (Jácome-Pilco et al. 2009). According to the World Health Organization, nickel is among the heavy metals of greatest and more immediate concern (Pahlavanzadeh et al. 2010). Divalent nickel [Ni(II)] is frequently encountered in raw wastewater streams from industrial processes such as nickel mining, metallurgy and electroplating, steel foundries and stainless steel production, electroforming and sintered metal coating production, non-ferrous metal, mineral processing, paint formulation, porcelain enameling, battery and accumulator manufacture, and steamelectric power plants (Pahlavanzadeh et al. 2010; Shroff and Vaidya 2011a; Suazo-Madrid et al. 2011). Although living organisms require trace amounts of Ni(II) for certain enzyme systems that participate in metabolic reactions such as ureolysis, hydrogen metabolism, methane biogenesis, and acidogenesis (Alomá et al. 2012), long-term exposure to high Ni(II) levels may

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cause acute and chronic health disorders such as skin dermatitis, allergic sensitization, gastrointestinal distress (nausea, vomiting, and diarrhea), pulmonary fibrosis, renal edema, and severe damage to the lungs, kidney, nervous system, and mucous membranes (Borba et al. 2006; Vinod et al. 2010). Besides, Ni(II) is carcinogenic and has been considered a nephrotoxic (Savolainen 1996), teratogenic, and embryotoxic agent (Pandey et al. 2007). Due to the deleterious effects of toxic Ni(II) ions on human and environmental health, it has become essential to remove them from industrial wastewater and from surface and ground water streams. In past years, Ni(II) ions have been removed by conventional treatments such as adsorption on activated carbon, ion exchange, chemical precipitation, and crystallization in the form of nickel carbonate (Malkoc 2006; WHO 2011). These methods, however, have several drawbacks such as high installation and operation costs, preliminary treatment requirements, generation of toxic sludge, poor efficiency at low Ni(II) concentrations (of less than 100 mg/L), and unpredictable metal ion removal (Shroff and Vaidya 2011a). Low cost, efficient, and secure technologies to remove Ni(II) ions from aqueous solutions are therefore crucial. Biosorption—the ability of certain biomaterials to bind and concentrate heavy metals, even from diluted aqueous solutions—offers a technically feasible and economical alternative to remove heavy metals from i n d u s t r i a l w a s t e an d n a t u r a l w a t e r s t r ea m s (Pahlavanzadeh et al. 2010; Serencam et al. 2013). The capacity to biosorb Ni(II) from aqueous solutions has been analyzed in some microorganisms as well as in biomaterials such as agroindustrial, forestry, and fishery by-products and biowastes (Gialamouidis et al. 2009; Malkoc 2006; Pradhan et al. 2005; Suazo-Madrid et al. 2011; Vinod et al. 2010). The marine penaeid shrimp (Farfantepenaeus aztecus) is found abundantly along the Atlantic coast of USA and Mexico. The species is of great commercial value, with a global capture reported to FAO in 2011 of about 59942 t (FAO 2013). Shrimp head represents 44– 50 % of the whole shrimp (Gernat 2001; Ramírez-Cruz et al. 2003) and is mainly composed of proteins, chitin, lipids, and ash (Arvanitoyannis and Kassaveti 2008). Shrimp head is an abundant biowaste material from shrimp-processing industries (Arvanitoyannis and Kassaveti 2008; Begum et al. 2012) and is mostly thrown back into the open ocean or at ports or even in municipal landfills generating water and soil pollution

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(Ramírez-Cruz et al. 2003). A thorough literature review showed that shrimp head has not been examined as biosorbent material for the removal of Ni(II) or other heavy metal ions from aqueous solutions. The aim of this work was to evaluate the potential of shrimp head (SH) to biosorb Ni(II) ions from aqueous solutions. The influence of relevant parameters such as SH pretreatment, solution pH, contact time, and initial metal concentration on Ni(II) biosorption was investigated. In addition, the kinetics and isotherm of Ni(II) biosorption onto SH are described.

Material and methods Biosorbent preparation F. aztecus heads (SH) were obtained free from the local wholesale market. SH were first washed thoroughly with distilled deionized water and then oven-dried at 60 °C until they reached a constant dry weight. Subsequently, they were milled using a Glen Creston hammer mill and the resulting particles were screened using ASTM standard sieves. The fraction of particle size between 0.3 and 0.5 mm was used in the present Ni(II) biosorption experiments. The sieved biomaterial was stored in an airtight plastic container until used. Ni(II) solutions for biosorption experiments Ni(II) stock solution was prepared by dissolving a weighed quantity of analytical grade NiSO4⋅6H2O (J.T. Baker®, Mexico; purity>99.1 %) in distilled deionized water. Experimental solutions were obtained by diluting the stock solution containing 2 g/L Ni(II). Initial Ni(II) concentrations varied from 20 to 300±5 mg/L, and the pH of each Ni(II) solution was adjusted to the desired value with 0.1 N HCl or NaOH solutions. Kinetic Ni(II) biosorption studies and analytical method Batch biosorption dynamics were analyzed to determine the influence of SH pretreatment, solution pH, shaking contact time, and initial Ni(II) concentration on Ni(II) biosorption by SH from aqueous solutions. Each biosorption experiment was conducted by varying only one parameter (e.g., solution pH) and maintaining the other parameters constant (e.g., initial Ni(II) concentration, temperature, agitation, etc.). All experiments were

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conducted in 500-mL Erlenmeyer flasks containing 150 mL Ni(II) solution of known concentration and 1 g (dry weight)/L of SH. Throughout the course of the experiments, all Ni(II) solutions were maintained at constant pH (±0.1 unit) by periodic checking and adjusted with 0.1 N HCl or NaOH solutions when necessary. Flasks were agitated in an orbital shaker (Cole Parmer®) at 150 rpm constant shaking speed and 25± 1 °C. To investigate the influence of SH pretreatment on Ni(II) biosorption, SH biomass (50 g/L) was pretreated as follows: (a) soaking in either 0.1 or 1 N HCl solutions for 6 h at 25 °C; (b) soaking in 2 N CH3COOH for 6 h at 25 °C; (c) soaking in 1 N Na2CO3 for 24 h at 25 °C; (d) soaking in 1 N KOH for 24 h at 25 °C; (e) soaking in either 0.1 or 1 N NaOH solution for 24 h at 25 °C; and (f) boiling in 0.5 N NaOH for 15 min (Shroff and Vaidya 2011b; Vijayaraghavan et al. 2004, 2005; Yan and Viraraghavan 2000). Once treated, the SH biomass was thoroughly washed with distilled deionized water until pH of the washing water was constant and then dried at 60 °C for 24 h. Ni(II) biosorption experiments using unpretreated and pretreated SH were conducted with a synthetic Ni(II) solution at initial metal concentration of 200 mg/L, pH 7.0, and 25 °C. The quantitative effect of pretreatment on Ni(II) biosorption was evaluated in terms of a global index of behavior (ξ) (RojasRejón et al. 2011), which is defined later in this paper. Further batch experiments were carried out using the pretreated SH that exhibited the highest values of Ni(II) biosorption capacity and ξ. The influence of solution pH level on kinetic performance was explored in Ni(II) solutions containing 200 mg/L initial metal concentration and different pH value ranging from 3.0 to 7.0, at 25 °C. The effect of initial Ni(II) concentration was evaluated by varying the initial metal concentration in the range from 20 to 300 mg/L, at 25 °C. For the equilibrium biosorption experiments, the shrimp head biosorbent (1 g/L) was mixed with metal solutions of different initial Ni(II) concentrations (20– 300 mg/L). The solutions were shaken at 150 rpm, 25 °C, for 168 h to ensure biosorption equilibrium was reached. Biosorbent-free controls were run simultaneously and under exactly the same conditions as used for the Ni(II) biosorption experiments to check for glassware sorption and other potential side effects (metal precipitation, etc.). No measurable changes in Ni(II)

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concentration were detected in the biosorbent-free controls throughout this work, which indicates that the Ni(II) removal found with pretreated SH was due only to the biosorbent. Samples were collected at different experimental times and filtered through 1.6-μm filter paper (Whatman GF/A). The filtrates were then analyzed at 232 nm for Ni(II) concentration by atomic absorption spectrophotometry (SpectrAA220, Varian Inc.). The amount of Ni(II) biosorbed at time t by the unit mass (dry weight) of biosorbent, which represents the Ni(II) biosorption capacity, was determined by the following mass balance equation: qt ¼

V ðC 0 − C t Þ M

ð1Þ

In this expression, qt is the Ni(II) biosorption capacity (in milligram per gram) at any time t (in hour), Co is the initial Ni(II) concentration (in milligram per liter) at time to =0 h, Ct is the Ni(II) concentration (in milligram per liter) at t=t (in hour), V is the solution volume (in liter), and M is the dry weight of the biosorbent (in gram). The global index of behavior was defined as follows (Rojas-Rejón et al. 2011): Z t f  Z t f  qt dt − qt dt 0 0 control Zproblem  ξ ¼ 100 ð2Þ tf qt dt 0

control

where ξ is the global index of behavior for Ni(II) biosorption, (qt dt)control and (qt dt)problem are the time courses of the Ni(II) biosorption capacity in experiments conducted with unpretreated SH (control experiments) and with pretreated SH (test experiments), respectively, and tf is the total experimental time. The experimental curves represented by (qt dt)control and (qt dt)problem were integrated using GraphPad Prism software version 5.03 (GraphPad Software, Inc.). Positive values of the index indicate an improvement in Ni(II) biosorption as compared to the control (i.e., positive effect). On the other hand, negative values indicate a decrease in Ni(II) biosorption compared to the control (i.e., negative effect). Biosorption kinetics modeling In this work, the kinetics of Ni(II) biosorption data were analyzed using the pseudo-first-order and the pseudo-

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Environ Monit Assess (2014) 186:7987–7998

second-order models, which have been widely used to analyze and understand biosorption kinetics of heavy metals by different biosorbents (Febrianto et al. 2009; Ho and McKay 1999; Ho 2006; Vaguetti et al. 2008). The nonlinear expression of Lagergren’s pseudofirst-order model (Febrianto et al. 2009) is as follows:  qt ¼ qe1 1−e−k 1 t ð3Þ where qe1 and qt are the biosorption capacities (in milligram per gram) at equilibrium and at time t (in hour), respectively, and k1 is the rate constant of the pseudo-first-order adsorption (1/h). The pseudo-second-order model proposed by Ho and McKay (1999) can be written as follows: qt ¼

t 1 t þ k 2 qe2 qe2

The equilibrium distribution of Ni(II) ions between the liquid phase and the biosorbent was expressed in terms of a Ni(II) biosorption isotherm. The Langmuir and Freundlich isotherm models, which are most frequently used to analyze data for water and wastewater treatment applications, were used in the present work to analyze the experimental equilibrium data of Ni(II) biosorption. The Langmuir equation is expressed as follows: ð5Þ

where qmax is the maximum biosorption capacity of the biosorbent (in milligram per gram), qe is the equilibrium metal ion concentration on the biosorbent (equilibrium biosorption capacity, in milligram per gram), Ce is the equilibrium metal concentration in the solution (in milligram per liter), and b is the Langmuir biosorption constant (liter per milligram) related to the free energy of biosorption, which quantitatively reflects the affinity between the biosorbent and the sorbate (Mohan and Pittman Jr. 2006). The essential features of a Langmuir isotherm can be expressed in terms of a dimensionless constant

1 1 þ b C0

ð6Þ

where Co is the initial Ni(II) concentration (in milligram per liter) and b is the Langmuir biosorption equilibrium constant (in liter per milligram). The value of the parameter RL indicates whether an isotherm is unfavorable (RL >1), linear (RL =1), favorable (0

Nickel(II) biosorption from aqueous solutions by shrimp head biomass.

The present study evaluates the capacity of shrimp (Farfantepenaeus aztecus) head to remove toxic Ni(II) ions from aqueous solutions. Relevant paramet...
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