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Appl Water Sci (2017) 7:4351–4360 https://doi.org/10.1007/s13201-017-0580-y ORIGINAL ARTICLE Functionalized dithiocarbamate chelating resin for the removal 2+ of Co from simulated wastewater 1,2 2 2 1 2 • • • • • Xuewei Shi Linwei Fu Yanyang Wu Huiling Zhao Shuangliang Zhao Shouhong Xu Received: 6 April 2017 / Accepted: 14 June 2017 / Published online: 28 June 2017 The Author(s) 2017. This article is an open access publication Abstract Industrial wastewater that contains trace Introduction amounts of heavy metal ions is often seen in petrochemical industry. While this wastewater can not be directly dis- Wastewater with heavy metal ions has aroused great con- charged, it is difficult to treat due to the low concentration cern because of their general and specific toxic nature and of metal ions. Introducing chelating reagents into this other adverse effects on human life. To address this con- wastewater for selective ion adsorption, followed by a cern, various methods, such as chemical precipitation mechanical separation process, provides an appealing adsorption (Liu et al. 2015; Huisman et al. 2006;Ozverdi solution. Toward the success of this technology, the and Erdem 2006), adsorption (Cui et al. 2014a, b; Kang development of effective chelating resins is of key et al. 2008), ionic exchange (Zhang et al. 2015; Li et al. importance. In the present work, a chelating resin con- 2014; Xie et al. 2014; Gode and Pehlivan 2006), electro- taining amino and dithiocarbamate groups was reported for chemical treatment (Chen 2004; Heidmann and Calmano the removal of Co(II) metal ions in trace concentrations 2008; Nanseu-Njiki et al. 2009), coagulation and floccu- from simulated wastewater. By investigating the adsorption lation (El Samrani et al. 2008), flotation (Lundh et al. 2000; performance of the chelating resin at different solution pH Yuan et al. 2008), and membrane separation technique (Du values, adsorbent dosages, contact time, initial ion con- et al. 2014), have been proposed for the development of centrations, and adsorption temperatures, the maximum cheap and effective wastewater treatment technologies. adsorption capacity of the resin for Co(II) was identified to While each method has its own advantage for treating -1 -1 be 24.89 mg g for a 2 g L adsorbent dosage and a pH wastewater with different levels of metal ion concentra- value of 5. After four adsorption–desorption cycles, 97% of tions, adsorption is the commonly used one and it has been the adsorption capacity of the resin was maintained. The widely employed in industry to remove hazardous metal adsorption kinetics and thermodynamics were analyzed ions or other contaminants from wastewater. This is and discussed as well. probably because the adsorption process is cheap to operate and flexible to maintain, and it also generates a high quality Keywords DTC resin Co(II) removal Adsorption effluent, even when metal ions are in trace concentrations kinetics Wastewater in the feed wastewater (Fu and Wang 2011). Thus, many inorganic and organic adsorbents have been prepared or examined, including zeolites (Jovanovic et al. 2012; Padervand and Gholami 2013), clay minerals (Al-Jlil and & Shuangliang Zhao szhao@ecust.edu.cn Alsewailem 2009), fly ash (Gupta and Torres 1998), biosorbents (Kadirvelu et al. 2001), and activated carbon Department of Chemistry, East China University of Science (Machida et al. 2012). Generally, these adsorbents exhibit and Technology, 130 Meilong Road, Xuhui District, high adsorption capacity, but limitations such as high Shanghai 200237, China operational costs, low recyclability and the introduction of State Key Laboratory of Chemical Engineering, East China a large volume of additional contaminants, have also been University of Science and Technology, 130 Meilong Road, found. Therefore, intensive studies have been carried out to Xuhui District, Shanghai 200237, China 123 4352 Appl Water Sci (2017) 7:4351–4360 develop more efficient, environmental friendly and inex- simulated wastewater was presented. DTC molecular pensive adsorbents for the removal of heavy metal ions group can strongly bind with various heavy metal ions and from wastewater. Kongsuwan et al. (Kongsuwan et al. display high removal efficiency due to its strong tendency 2009) explored the use of activated carbon from eucalyptus of sharing electrons between N, S elements and heavy bark in a binary component adsorption of Cu(II) and Pb(II), metal ions (Bai et al. 2011). For example, Fan et al. and the maximum adsorption capacities achieved were (2014a, b, c) prepared three different silica-supported ion- -1 -1 0.45 mmol g for Cu(II) and 0.53 mmol g for Pb(II). imprinted hybrid sorbents all functionalized with S, Agoubordea and Navia (Agouborde and Navia 2009) N-donor atoms for lead (II), cadmium (II) and lead (II) investigated brine sediments, sawdust and the mixture of through the surface imprinting technique. The sorbents -1 both materials to remove Zn(II) or Cu(II) from aqueous showed high adsorption for Pb(II) (54.9 mg g ), Cd(II) -1 -1 solutions; the maximum adsorption capacities of these (29.1 mg g ) and Pb(II) (61.9 mg g ) within 30 min, three adsorbents were identified to be 4.85, 2.58 and respectively. In addition, Fan et al. (Fan et al. 2011) -1 -1 5.59 mg g for Zn(II) and 4.69, 2.31 and 4.33 mg g for presented a Co(II)-imprinted silica gel sorbent with the Cu(II), respectively. Gao et al. (Gao et al. 2009) investi- same technique as mentioned above and the maximum -1 gated anion removal from aqueous solutions using grafting adsorption capacities toward Co(II) was 35.2 mg g -1 particles PEI@SiO , and a high saturated adsorption compared to 6.5 mg g which is the non-imprinted. 2- -1 amount for CrO ions of up to 0.14 g g was reported, Hence, micromolecular DTC is usually synthesized from owing to electrostatic interactions. carbon disulfide and amino compounds, including The removal of Co(II) from industrial wastewater is diethylenetriamine, triethylenetetramine, ethylenediamine, demanded in petrochemical plants, where Co(II) comes diethylamine, etc., under an alkaline environment (Stathi primarily from the utilization of metal catalysts for the et al. 2010; Jones et al. 1980; Shaaban et al. 2013; Horvath production of chemical raw materials such as pure and Barnes 1986). However, many limitations have also terephthalic acid. The concentration of Co(II) in initial been found, such as being volatilizable, very expensive, -1 wastewater is readily high up to 2.0 g L . After prelimi- not easily available, and toxic (Talebi et al. 2010; Ling nary treatment with sedimentation, the ion concentration et al. 2011). To tackle these problems, the DTC resin here can be reduced by up to 90%. However, the resultant was developed by grafting polyethyleneimine (PEI) onto concentration of Co(II) is still much beyond the effluent chloromethylated polystyrene (CPS) beads (Gao et al. -1 standard in China, namely 1.0 mg L (National Standards 2006) as the amino compound. To examine the adsorption of Integrated Wastewater Discharge Standard, People’s capability, different simulated wastewater bodies with Republic of China 1996). The pre-treated wastewater is various Co(II) concentrations in the range of -1 usually recycled by mixing with fresh water for the purpose 40–320 mg L were tested. The maximum adsorption of energy-saving and emission reduction. Nevertheless, the conditions of Co(II) have been identified and the nature of recycling of wastewater that contains even trace amounts the adsorption process with respect to its kinetics and of heavy metal ions causes several troublesome problems. thermodynamic aspects were investigated. First, the deposition of heavy metal ions in biochemical ponds gradually reduces the biological activity of bacteria, and thereafter depresses the degradation efficiency of Experimental ´ ´ organic contaminants (Mathe et al. 2012). Second, charged metal ions have a strong tendency to associate with many Materials and instruments membranes utilized for filtration, causing membrane foul- ing (Zhao et al. 2016). Third, the presence of metal ions in Chloromethylated polystyrene beads were purchased from feed wastewater can result in serious corrosion of metal the Chemical Plant of Nan Kai University (Tianjin, China), devices through an ion-exchange process. Whereas it is and polyethyleneimine was purchased from Sigma Aldrich relatively easy to reduce the concentration of heavy metal Co. (USA). Carbon disulfide, sodium hydroxide, chloro- ions from a high value to a low one, the removal of trace form, and alcohol were purchased from General Chemical amounts of heavy metal ions from wastewater is much (Shanghai, China). All other reagents were of analytical more challenging. Introducing chelating reagents for ion grade and used as received. All solutions were prepared adsorption, followed by a mechanical separation process, with ultrapure water. provides one promising solution. The realization of this In the ion adsorption experiments, the pH values of the method highly relies on the development of excellent aqueous solutions were measured using a Hanna HI221 chelating reagents. model pH meter, and the temperature-dependent experi- In this work, a dithiocarbamate (DTC) resin prepared as ments were carried out in a Nickel Electro Clifton NE1-22 a novel adsorbent for the removal of Co(II) from model thermostatic bath. The concentration of Co(II) ions 123 Appl Water Sci (2017) 7:4351–4360 4353 was measured using a Perkin-Elmer Analyst 200 model Adsorption studies atomic absorption spectrophotometer (AAs). All of the adsorption experiments, including pH effect, Synthesis and characterization adsorbent dosage, kinetic and isotherm study, were con- ducted batch-wise. -1 The synthesis procedure of the chelating resin involved A 320 mg L (320 ppm) stock solution of Co(II) was prepared by dissolving CoCl 6H O in ultrapure water. three steps: 2 2 Solutions with different Co(II) concentrations in a range of (i) 10.0 g of the CPS beads was added into 50 ml of -1 40–320 mg L were prepared by diluting the stock solu- chloroform in a round-bottom flask, and the resultant tion. Adsorption experiments related to pH and adsorbent suspension was stirred at 600 rpm at 25 C for 12 h. dosage effect were performed at 25 C in the thermostatic Afterward, the swollen CPS beads were washed with bath. To determine the effect of pH value, adsorption alcohol and ultrapure water three times and then experiments were carried out at different pHs in a range separated from the supernatant by filtration; -1 from 1 to 5 by mixing 100 ml of 80 mg L aqueous (ii) 4.0 g of sodium hydroxide was dissolved in 100 ml Co(II) solutions with 0.2 g of adsorbent. The pH values of of ultrawater, and 10 g of PEI was added to this the initial solutions were adjusted by adding dilute NaOH solution. Then, the pretreated CPS beads were added or HCl solutions. To assess the optimal adsorbent dosage, to the solution and the mixture was stirred at 600 rpm -1 100 ml 80 mg L aqueous Co(II) solutions were mixed at 50 C for 15 h; with varying amounts of adsorbent in a range of 0.2–1.0 g (iii) The pretreated CPS beads carrying the PEI were at pH 5. added into a mixture of 100 ml of ultrawater, 10 ml The adsorption isotherms were evaluated through a of carbon disulfide and 4 g of sodium hydroxide. The series of adsorption measurements at three different tem- resultant mixture was stirred at 600 rpm at 20 C for peratures (20, 30 and 40 C) and different initial Co(II) ion 12 h, continuously at 50 C for another 12 h. The -1 concentrations in the range of 40–320 mg L at pH 5. To obtained product was washed individually with water achieve adsorption equilibrium, the adsorption time was and ethanol; then, it was dried in a vacuum oven at extended to 24 h in these experiments. The Co(II) ion room temperature, milled, and sieved for utilization concentration was monitored using an atomic absorption in the adsorption experiments. spectrophotometer in the adsorption experiments, and then -1 Figure 1 showed the FT-IR spectra of DTC chelating the adsorption capacity, i.e., q (mg g ), of the adsorbent -1 resin. The adsorption peaks at 1617 and 1300 cm stand was calculated as for C=N and C–N stretching vibrations. The peak at -1 ðÞ C C V 0 e 3363 cm is caused by the N–H stretching vibrations, and q ¼ ; ð1Þ -1 the characteristic peak at 1071 cm is attributed to C=S stretching vibrations, indicating that DTC functional group where C and C are, respectively, the initial and final 0 e -1 is attached to the resin. concentrations of Co(II) ions in the solution (mg L ); V is the volume of the solution (L) and m is the weight of the adsorbent (g). All assays were carried out in triplicate and only the average values were presented. The removal efficiency (Re %) of the resin was calculated using the following conventional equation: Re% ¼ðC C Þ=C 100%: 0 e 0 The kinetic studies were carried out at 25 C, and the initial metal ion concentration, adsorbent dosage and the pH of the adsorption solutions were chosen to be -1 80 mg L , 0.2 g/100 ml, and 5, respectively. 3363 Desorption and regeneration assay 4000 3500 3000 2500 2000 1500 1000 500 The desorption of metal ions adsorbed on the resin was -1 Wavenumber (cm ) performed by the agitated mixing of 0.2 g of Co(II)-loaded -1 resins and 20 mL of 0.1 mol L HCl solution at room Fig. 1 FT-IR spectra of DTC chelating resin Transmitance (%) 4354 Appl Water Sci (2017) 7:4351–4360 temperature for 4 h. After filtration, the final metal ion Results and discussions concentrations in the aqueous solution were determined by AAs. The desorption ratio (De %) was calculated by Effects of pH and adsorbent dosage dividing the amount of heavy metal ion desorbed into the acid medium by the total amount adsorbed onto the DTC- It has been reported that the pH value alters the metal chelating resin. chemistry in a solution or the protonation or deprotonation After the desorption process, the collected DTC resin of the adsorbents (Bayramoglu et al. 2002). Figure 3 was washed thoroughly three times with ultrapure water showed the effects of pH and dosage on the adsorption of and then dried in a vacuum for the next adsorption test. To Co(II). First, it was clearly seen that the affinity of resin access the reusability of the DTC resin, the adsorption– towards Co(II) was sensitive to the pH value. When the pH desorption cycles were repeated four times by using the decreased, the adsorption capacity became smaller. This is same affinity adsorbent. likely due to the competitive adsorption of H ions with Figure 2a–c displayed the simulated wastewater after 0, Co(II) on the same active site. This finding coincides with 60 and 120 min with the introduction of DTC resin, and the previous studies (Liu et al. 2006; An et al. 2011). When the temperature, initial metal ion concentration, adsorbent pH value was higher than 5, Co(II) might have the dosage and the pH of the adsorption solutions were 25 C, hydrolysis reaction and lead up to the hydroxyl complexes, -1 80 mg L , 0.2 g/100 ml, and 5, respectively. Apparently, resulting in a lower adsorption capacity. Because the pH of the adsorption of Co(II) ion has bleached the color of industrial wastewater is approximately 5, we adopted the simulated wastewater. Figure 2d–f presented the DTC simulated wastewater with pH = 5 in the following studies resins before and after the usage of wastewater treatment. It (unless it was specified otherwise). Second, the curve of the was seen that the yellow DTC resins became green after adsorption capacity as a function of the adsorbent dosage adsorbing Co(II) ions. showed that, when more dosage was added, the adsorption Fig. 2 Simulated wastewater after a 0, b 60 and c 120 min with the addition of DTC resin; the prepared DTC resins d before and e after the usage for wastewater treatment and f after four desorption–adsorption circles 123 Appl Water Sci (2017) 7:4351–4360 4355 Fig. 3 Effects of pH value (a) 30 (b) 28 (a) and adsorbent dosage (b)on Re=61.61% the adsorption of Co(II) onto the 25 DTC resins Re=70.23% Re=78.69% Re=84.33% Re=87.46% 1234567 0.2 0.4 0.6 0.8 1.0 pH of initial solution m (g) capacity decreased; meanwhile, the removal efficiency Table 1 The maximum adsorption capacity of Co(II) ion in different adsorbents increased, indicating that a tradeoff between adsorption capability and removal efficiency should be considered in Adsorbent q (mg/g) Refs. practical usage. Lemon peel 22 Bhatnagar et al. (2010) Almond green hull 10.22 Ahmadpour et al. (2009) Adsorption kinetics Magnetite silicate composite 9.4 Ebner et al. (2001) Kaolinite 1.74 Yavuz et al. (2003) Contact time is a crucial parameter directly associated with Sepiolite 7.57 Kara et al. (2003) the design and operation of a separation technology. Fig- DTC resin 24.89 This work ure 4 showed the adsorption capacity of Co(II) as a func- tion of contact time onto the DTC resin. During the initial 1-h adsorption period, the adsorption capacity, q , pre- To clarify the kinetic characteristics of the adsorption, sented a sharp increase with increasing contact time, different kinetic models were adopted to analyze the reaching a plateau after almost 3 h. Specifically, within the experimental data in this work. We found that the -1 first hour, q reached 19.87 mg g (79.8% of the total adsorption kinetics could be well described with the adsorption); at 3 h, more than 97% of the total adsorption pseudo-second-order kinetic model, which is given by the -1 was completed, and q was found to be 24.14 mg g . equation (Ho and McKay 1999). After 3 h, the adsorption rate slowed down and, after 5 h, t 1 t reached equilibrium, while the maximum of q was found ¼ þ ; ð2Þ -1 2 q Kq q to be 24.89 mg g . t e Table 1 presented the maximum adsorption capacity of -1 -1 where K (g mg min ) is the rate constant of the pseudo- Co(II) ion in different adsorbents. Apparently, the second-order adsorption reaction. A second-order kinetic adsorption capacity of DTC resin was very competitive. can be applicable if the plot of t=q versus t shows linearity. Figure 5 showed the plots obtained from the graphical interpretation of the data for the second-order kinetic model, as well as the corresponding fitting parameters -1 K = 0.00268 and q = 25.3 mg g . In addition to the very high correlation coefficient of the fitting curve (R ¼ 0:9998), the excellent accordance -1 between experimental (24.89 mg g ) and theoretical -1 10 (25.3 mg g ) q values confirms that the adsorption of Co(II) metal ions onto the DTC resin follows pseudo-sec- ond-order type reaction kinetics. It is generally understood that pseudo-second-order kinetics provide the best fits to the experimental data for the adsorption systems where 0 200 400 600 800 1000 1200 1400 1600 chemisorption seems significant in the rate controlling step t (min) (Ho and McKay 1999; Zheng and Wang 2010); therefore, for our DTC resin, the chemisorption should be the rate Fig. 4 Effect of contact time on the adsorption of Co(II) ion onto the determining step in the adsorption process. DTC resin -1 q (mg g ) q (mg/g) q (mg/g) e 4356 Appl Water Sci (2017) 7:4351–4360 70 C 1 C e e ¼ þ ð3Þ q bq q e max max The linear form of the Freundlich equation is given as (Freundlich 1906). ln q ¼ ln K þ ln C ; ð4Þ e f e 30 n where q is the monolayer capacity of the adsorbent max -1 -1 (mol g )and b is the Langmuir constant (L mol ) related to the free energy of adsorption; K is the Freundlich constant and n is the indicator of adsorption intensity. The plots of Lang- muir adsorption at the three temperatures are shown in Fig. 7. 0 400 800 1200 1600 The parameters and correlation coefficients obtained from t (min) these plots are listed in Table 2. For all temperatures, the Langmuir correlation coefficients are closer to 1 than Fre- Fig. 5 Pseudo-second-order kinetics plots for the adsorption of undlich, suggesting that Co(II) adsorption on the adsorbent Co(II) onto the chelating resin can be interpreted using the Langmuir adsorption model. The adsorption capacity of an adsorbent was represented Adsorption isotherm as q . As seen from Table 2, q increased with max max increasing temperature, indicating the endothermic nature The removal of Co(II) by the DTC resin as a function of the of the adsorption process. In addition, the favorability of initial concentration was studied at three typical tempera- the adsorption process can be determined by the separation tures (20, 30, 40 C) while varying the ion concentration -1 constant, i.e., R (Namasivayam and Ranganathan 1993; from 40 to 320 mg L , keeping all other parameters Dalaran et al. 2009), which is defined as constant. The results were displayed in Fig. 6. It was shown that q values tended to increase significantly with 1 R ¼ : ð5Þ the increase of the initial Co(II) concentration. In addition, 1 þ bC a higher temperature results in a bigger q , indicating that For all initial metal ion concentrations in the range of the adsorption of Co(II) onto the resin is an endothermic -1 40–320 mg L , the R values were found to be between 0 process. and 1.0, which indicated that the adsorption of Co(II) onto There are two most generally used isotherms, namely the DTC resin was a favorable adsorption. The R values Langmuir and Freundlich adsorption isotherms. We found are listed in Table 2. It was clear that a higher temperature that the adsorption isotherm could be analyzed with the resulted in a higher R value, showing that adsorption was Langmuir adsorption model. The linear form of the more favorable at lower temperatures. Langmuir equation is given as (Langmuir 1918). The adsorption mechanism can be suggested by the mean energy of adsorption; the latter refers to the free 293K 303K 313K 0 50 100 150 200 250 -3 -1 -1 C (×10 mol L ) C (mg L ) Fig. 6 Effect of initial ion concentration on the adsorption of Co(II) Fig. 7 Langmuir plots for the adsorption of Co(II) onto the DTC onto the DTC resin resins at different temperatures -1 -1 q (mg g ) t/q (min.g.mg ) -1 C /q (g L ) e e Appl Water Sci (2017) 7:4351–4360 4357 Table 2 Isotherm constants for the adsorption of Co (II) onto the resin at different temperatures T(K) Langmuir equation Freundlich equation D-R equation -3 3 3 1-1/n 2 -3 -3 -1 q (10 b(10 L R K (10 mol 1/nR q (10 b(10 E (KJ mol ) max L f m a -1 -1 1/n -1 -1 2 2 mol g ) mol ) L g ) mol g ) mol kJ ) 293 0.5016 3.7565 0.9943 0.0520 0.3596 0.1977 0.9917 0.7 1.8310 16.5248 303 0.5637 3.2799 0.9955 0.0531 0.4005 0.2165 0.9769 0.9 1.8810 16.3038 313 0.6654 2.9331 0.9938 0.0571 0.4515 0.2501 0.9833 0.11 1.9725 15.9212 energy change when transferring one mole of adsorbate an adsorption process. According to values of these from the bulk solution to the surface of the adsorbent, and parameters, the spontaneously occurring process can be pffiffiffiffiffiffi determined. The thermodynamic data were calculated from it can be calculated (Hobson 1969)as E ¼ 1= 2b. Here, 2 -2 the Langmuir isotherms using the following equations: b (mol kJ ) is the constant in the Dubinin–Radushkevich (D-R) (1947) isotherm equation 0 DG ¼R T ln b; ð7Þ ln q ¼ ln q be ; ð6Þ e m T T b 2 1 2 DH ¼R ln ; ð8Þ T T b where q is the theoretical saturation capacity; e is the 2 1 1 Polanyi potential, which is equal to R T lnð1 þ 1=C Þ, with c e 0 0 DH DG -1 -1 R (J mol K ) being the gas constant and T (K) the DS ¼ ; ð9Þ absolute temperature. The two parameters q and b can be where b and b are the Langmuir constants [or, equiv- 1 2 obtained by fitting the experimental adsorption isotherm alently, b in Eq. (7)]at temperatures T and T , respec- 1 2 curves in Fig. 5. Both parameters, together with the tively. b at three different temperatures are listed in thereafter calculated mean energies of adsorption, are Table 2. presented in Table 2. The thermodynamic properties for the present adsorp- It is said that when the value of E is in the range of 1– -1 tion systems at three different temperatures are given in 8 kJ mol , it corresponds to a process dominated by -1 0 Table 3. As shown, the DG value was negative, and it physical adsorption; in the range of 8–16 kJ mol decreased slightly with increasing temperature, indicating (Onyango et al. 2004; Helfferich 1962), it corresponds to a the spontaneous nature of the adsorption process and a process dominated by an ion-exchange mechanism. In -1 more spontaneous tendency at higher temperatures. Gen- Table 2, E values were higher than 16 kJ mol at 293.15 erally, the Gibbs free energy for a physisorption is in the and 303.15 K, which indicates that neither physical -1 range of -20 to 0 kJ mol ; however, that for a adsorption nor an ion-exchange mechanism is the dominant chemisorption is much lower, in the range of -80 to factor, and another mechanism with an even stronger effect -1 -400 kJ mol (Donia et al. 2006). The values of DG in on the adsorption should be accounted for. Considering the DTC and amino functional groups on the resin surface, the the present work were slightly lower than that of a physisorption, but much higher than that of a chemisorp- adsorption of Co(II) occurs through electrostatic attraction, ion-exchange, and chelating mechanisms, simultaneously. tion, suggesting that both the physisorption and chemisorption mechanisms occur in the adsorption process. Thus, by excluding the physical adsorption and ion-ex- change mechanisms as the dominating factors, it is safe to Thus, a mechanism combining chelation and ion exchange took place during the process, coinciding with the above deduce that the chelating mechanism has a dominant effect kinetics analysis and isotherms models studies. Finally, a on Co(II) adsorption on the resin. However, the value of E -1 at 313.15 K dropped into the range of 8–16 kJ mol , positive DH suggests an endothermic reaction. indicating that the ion-exchange mechanism takes over the dominant position. This is because, at high temperatures, ion-exchange becomes relatively more favorable than Table 3 Thermodynamic parameters for the adsorption of Co(II) chelating. onto the DTC resin -1 -1 -1 -1 0 0 0 T (K) DG (kJ mol ) DH (kJ mol ) DS (kJ mol K ) Adsorption thermodynamics 293.15 -20.052 – – Thermodynamic parameters, including changes in the 303.15 -20.389 3.9392 0.08012 0 0 Gibbs free energy (DG ), enthalpy (DH ), and entropy 313.15 -20.777 – – (DS ), are the actual indicators for practical application of 123 4358 Appl Water Sci (2017) 7:4351–4360 Table 4 The adsorption capacities and the desorption ratios of the parameters clearly indicate that the ongoing adsorption DTC resin after different adsorption–desorption cycles process is feasible, spontaneous, and endothermic in nat- -1 ure. Desorption and reuse experiments showed that the Cycle q (mg g ) Desorption (%) dithiocarbamate resin could be used at least four times 1 24.89 99.1 without any significant loss in the adsorption performance. 2 24.80 98.7 All of these findings indicate that the dithiocarbamate resin 3 24.72 98.1 can be used as an effective adsorbent for the removal of 4 24.60 97.3 Co(II) from aqueous solutions. Acknowledgements This work is supported by the National Basic Research Program of China (2014CB748500), the National Natural Desorption and regeneration study Science Foundation of China (No. 91434110), the 111 Project of China (No. B08021) and the Fundamental Research Funds for the The discussion of pH effect on the adsorption capacity Central Universities of China. YW also acknowledges the support of suggested that desorption of the adsorbed cobalt ions on the Shanghai Pujiang Program (Grant No. 16PJD019). chelating resin can be easily performed in an acidic solu- Open Access This article is distributed under the terms of the tion. A similar study (Say et al. 2006) also reported the Creative Commons Attribution 4.0 International License (http:// effectiveness of acidic conditions on the desorption of creativecommons.org/licenses/by/4.0/), which permits unrestricted adsorbed metals. Therefore, the desorption was performed use, distribution, and reproduction in any medium, provided you give -1 appropriate credit to the original author(s) and the source, provide a in a 0.1 mol L HCl solution. As seen in Table 4, the link to the Creative Commons license, and indicate if changes were chelating resin had its largest initial adsorption capacity made. during the first cycle. The De % of the chelating resin was found to be 99.1% after the first cycle and then gradually decreased to 98.7, 98.1 and 97.3% for the second, third and References fourth cycles, respectively. It was observed that the Co(II) adsorption capacity of the resin did not show a significant Agouborde L, Navia R (2009) Heavy metals retention capacity of a non-conventional sorbent developed from a mixture of industrial loss for each repeated adsorption–desorption cycle, and the and agricultural wastes. J Hazard Mater 167(1–3):536–544 adsorption capacity of the resin for the fourth adsorption Ahmadpour A, Tahmasbi M, Bastami TR et al (2009) Rapid removal -1 was found to be 24.60 mg g , which indicates approxi- of cobalt ion from aqueous solutions by almond green hull. mately a 4% loss of adsorption capacity from the initial J Hazard Mater 166(2–3):925–930 Al-Jlil SA, Alsewailem FD (2009) Saudi Arabian clays for lead use. 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Applied Water Science – Springer Journals
Published: Jun 28, 2017
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