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ScienceDirect Materials Today: Proceedings 5 (2018) 21698–21702
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The 3rd International Conference on Green Chemical Engineering Technology (3rd GCET_2017): Materials Science
Selective recovery of Copper from waste mobile phone printed circuit boards using Sulphuric acid leaching Md. Sohrab Hossain*, Ahmad Naim Ahmad Yahaya, Lily Suhaila Yacob, Mohd Zulkhairi Abdul Rahim, Nor Nadiah Mohamad Yusof, Robert Thomas Bachmann Green Chemistry & Sustainable Technology Cluster, Universiti Kuala Lumpur-Malaysian Institute Chemical & Bioengineering Technology, 78000 Alor Gajah, Malacca, Malaysia.
Abstract In the present study, the leaching of Cu(II) from the waste mobile phone printed circuit board (WM-PCB) was investigated using concentrated sulphuric acid solution. Cu(II)) uptake efficiency was determined at varying pH (pH 2.0 – pH 8.0), temperatures (40 o C-80 oC) and treatment time (15 - 90 min). It was observed that the copper uptake increased with increasing temperature and acid concentration. The highest Cu(II) uptake was found to be 190 mg/g at pH 6.0 and 80oC within 60 min. Results indicate that sulphuric acid has the potential to recover the heavy metals from WM-PCB. © 2018 Elsevier Ltd. All rights reserved. Selection and/or Peer-review under responsibility of The 3rd International Conference on Green Chemical Engineering and Technology (3rd GCET): Materials Science, 07-08 November 2017. Keywords: Acid leaching; Printed circuit boards; Waste mobile phones; Copper recovery.
1. Introduction 1. Introduction Mobile phones are the most used electronic devices in worldwide, resulting the generation huge amount used mobile phone waste. As the mobile phone companies manufactures new mobile phones with the advanced technologies, Mobile phones are the mostphones used electronic in worldwide, resulting the generation huge [1, amount used mobile the number of used mobiles rises and devices along with the huge amount of discarded old phones 2]. Mobile phones phone waste. As the mobile phone companies manufactures new mobile phones[2]. with the advanced technologies, the contain hazardous substances, thereby increasing concern of their safe disposal Generally, a mobile phone consist of a printed circuit board (PCB), liquid display matter, a battery[1, and [3]. number of used mobiles phones crystal rises and along with (LCD), the hugeantenna, amountpolymeric of discarded old phones 2].keyboard Mobile phones contain hazardous substances, thereby increasing concern of their safe disposal [2]. Generally, a mobile phone consist of a printed circuit board (PCB), crystal liquid display (LCD), antenna, polymeric matter, a battery and keyboard [3]. The PCB contains huge amount of valuable metals such as copper (Cu), zinc, iron, nickel, aluminum, *Corresponding author. Tel: +606 551 2155; Fax: +606 551 2001 Email address:
[email protected] (M.S. Hossain).
2214-7853 © 2018 Elsevier Ltd. All rights reserved. Selection and/or Peer-review under responsibility of The 3rd International Conference on Green Chemical Engineering and Technology (3rd GCET): Materials Science, 07-08 November 2017.
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The PCB contains huge amount of valuable metals such as copper (Cu), zinc, iron, nickel, aluminum, gold, silver, and palladium [2,3]. The natural resources of these valuable metals are extremely limited rendering the recovery of these valuable metals from waste mobile phone PCBs (WM-PCBs) crucial to have raw materials with minimize environmental impact [4]. Studies reported that the WM-PCBs contains 15-38% copper, depending on the source and type of the circuit board [3, 7-9]. Hagelüken [9] recycled 130 kg of Cu(II )from one ton of WM-PCBs. Owing the high concentration, the recovery of Cu(II)from the WM-PCBs is bearing considerable economic potential. At present the heterogeneous and complex structure of WM-PCBs is the main obstacle to recovery metals from it. Many studies have been conducted to selectively recover valuable metals from WM-PCBs. At present the most economical recovery appears to be based on the hydrometallurgical process [2, 6]. The hydrometallurgical process is mostly conducted using concentrate acid and alkaline solutions to leach out the solid material followed by purification [2]. The most common leaching agents are aqua regia, cyanide, thiourea, halide, and thiosulfate [2, 3, 8, 9]. Although aqua regia and cyanide have promising recoveries of metals from WM-PCBs, these leaching agents are very toxic and raised concern occupational safety and environmental pollution issues [4, 8]. The use of sulphuric acid as a leaching agent to recover metals from WM-PCBs could be an alternative acid, since sulphate ion possess a high affinity for metal ions (reference). Further, the utilization of sulphuric acid as a leaching agent would be more economic, as sulphuric acid is cheaper than aqua regia and cyanide. The present study therefore aims to determine the possibility of sulphuric acid to be used as an effective alternative leaching agent for the recovery of Cu(II) from WM-PCBs. 2. Materials and Methods 2.1. Sample Preparation The WM-PCB was collected from a mobile repair shop, Tampin, Negri Sembilan, Malaysia. The polymeric materials from the collected WM-PCB were removed and cut into small pieces mechanically. Subsequently, it was ground into ≤ 200 mesh using mechanical cutting (Retsch, model SM2000). 2.2 Leaching of Cu(II)from WM-PCB The leaching of the WM-PCB was carried out using sulphuric acid (supplier, grade) at various pHs (pH 2.0-pH 8.0), temperatures (40oC – 80oC) and acid concentrations (0.1 M- 0.1.0 M) for leaching time of 15 min – 90 min. A 1 g ground WM-PCB was transferred into 100 mL of desired concentration of H2SO4 and stirred on a magnetic stirrer (manufacturer, grade?). At the end of the leaching process, the WM-PCBs was separated from the mixture using a Whatmann filter paper. The Cu(II) concentrations in the aqueous phase were measured by atomic absorption spectrophotometer after dilution with 0.1 M HNO3. The pH value of the aqueous solution was adjusted with H2SO4 or NaOH solution, the temperature was controlled using a thermostated bath (manufacturer, model). The amount of Cu(II) recovered from leaching was calculated as below.
C m Cu
m Cu V ( mg ) C V
(1) (2)
(1) (2)
m Cu (3) (3) m PCB where C is Cu(II) concentration in the aqueous solution (mg/L), V is the volume of the acid solution (mL), mCu is the mass of the Cu(II) (mg) and mPCB is the mass of the WM-PCB (mg). Cu recovered from WM - PCB (mg/g)
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3. Results and Discussion
The pH plays an effective role on the metal separation and recovery. Thus, it is important to determine the influence of pH on Cu(II) removal from WM-PCBs. The recovery of Cu(II) from WM-PCB was conducted with varying pH from pH 2.0 – pH 8.0 at constant acid concentration 0.5 M, temperature 60 oC for 15 min -90 min, as presented in Fig. 1. It was observed the Cu(II) recovery increased with increasing pH from pH 2.0 to pH 6.0, thereafter the Cu(II)recovery decreased with further increased of pH. The observed drop may also be due to the formation of copper hydroxide complexes with low Ksp. In the case of leaching time, the Cu(II) recovery slightly increased with increasing temperature below the pH 4 (in high acidic region). Wherein, the Cu(II) recovery increased with increasing temperature over the pH 4.0 up to 75 min, thereafter the increased of the Cu(II) removal was negligible. The optimal Cu(II) recovery was gained about 190 mg/g at pH 6.0, temperature 60 oC and leaching time of 75 min.
Recovery of Copper, mg/g
200
pH 2.0 pH 5.0 pH 8.0
160
pH 4.0 pH 6.0
120 80 40 0 0
15
30
45
Time, min
60
75
90
Fig. 1. Effect of pH with varying leaching time on the Cu(II)recovery of from waste mobile phone printed circuits board. Experimental conditions, Temperature 60 oC, acid concentration 0.5 M.
Temperature greatly affects the leaching kinetics of copper removal from PCBs [8].Cu(II) recovery was prominently influenced with temperature and leaching time, as presented in Fig.2. It was found that the Cu(II) removal increased with temperature 40 oC to 80 oC. The highest Cu(II) removal was obtained about 138 mg/g at 40 o C for 90 min leaching time, which was enhanced to 192 mg/g at temperature 80 oC for the similar leaching time. Chen et al. [10] observed that the leaching velocities were appreciably lower below the room temperature, above the room temperature leaching of Cu(II) increased with temperature and leaching time.
Recovery of Copper, mg/g
200
40 oC 60 oC 80 oC
160 120 80 40 0 0
15
30
45
60
75
90
Time, min Fig. 2. Effect of temperature with varying leaching time on the Cu(II)recovery of from waste mobile phone printed circuits board. Experimental conditions, pH 5.0, acid concentration 0.5 M.
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The influence of sulphuric acid concentration with varying leaching time on the removal Cu(II) from WM-PCBs, as presented in Fig.3. It was found that Cu(II) removal increased with increasing acid concentration and leaching time. In the case of acid concentration, the Cu(II) removal increased with increasing acid concentration from 0.1 M to 0.5 M, thereafter the increased of Cu(II) removal was found negligible with the further increased of acid concentration. Further, the Cu(II) removal was minimal with increasing acid concentration below 30 min leaching time. However, the Cu(II)recovery gradually increased with increasing leaching time 15 min to 90 min for acid concentrations of 0.1 M and 0.2 M. In the case of acid concentration over 0.2 M, the Cu(II) removal increased with increasing leaching time up to 75 min, thereafter there increased of the Cu(II)removal was observed negligible with further increase of leaching time. Similarly, studies reported that acid concentration pronounces the metal recovery from the waste printed circuit board [2,7]. For instance, Jha et al. [2] found that the lead recovery increase with acid concentration up to 0.4 M and decreased with further increase of the acid concentration.
Recovery of Copper, mg/g
200 160
0.1 M
0.2 M
0.5 M
1.0 M
120 80 40 0 0
15
30
45
60
75
90
Time, min Fig. 3. Effect of acid concentration with varying leaching time on the Cu(II)recovery of from waste mobile phone printed circuits board. Experimental conditions, Temperature 60 oC and pH 5.0.
The widespread utilization of mobile phone are generating huge amount WM-PCBs, after it has discarded due to its short life span. Thus, determination of effective treatment method for the safe disposal of this waste is essential in order to preserved human health and environment. It was found from the study that sulphuric acid could be utilized to recovery valuable metals from WM-PCBs. The optimal Cu(II) recovery was obtained about 190 mg/g (19 wt%) at pH 5.0 and 80 oC for 90 min leaching time, which lower than study conducted by Petter et al. [3]. Petter et al. [3] characterized heavy metal content in WM-PCBs by digesting WM-PCBs with aqua regia at 80 oC for 120 min. The study reported the Cu(II)content in aqua regia digested WM-PCBs is about 35.5 wt% [3]. The variation of the result obtained in the present study might due to the variation of experimental conditions and utilized aqua regia as a leaching agent, which is considered as the strongest chemical dissolver [4]. However, the utilization of aqua regia as leaching agent may arise environmental pollution due to its toxicity. Thus, the sulphuric acid can be considered as an alternative leaching agent to recover valuable metals from WM-PCBs. 4. Conclusion
The present study was conducted to determine the possibility of Cu(II) recovery from WM-PCBs using sulphuric acid as a leaching agent. The findings of the present study revealed that sulphuric acid could be utilized as leaching agent to recover valuable metals from WM-PCBs. The optimal Cu(II) recovery was obtained about 190 mg/g at pH 5.0 and 80 oC for 90 min leaching time. However, it urge to conduct further study on kinetics behaviour of sulphuric acid leaching, simultaneous recovery of Cu(II) with other valuable metals and optimized the experimental
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conditions in order to obtained maximum recovery of heavy metals from WM-PCBs using sulphuric as a leaching agent. Acknowledgements
The authors are greatfull to Universiti Kuala Lumpur- Malaysian Institute Chemical & Bioengineering Technology for the financial support. References [1] H. Wieser and N. Tröger, Journal of Cleaner Production, (2017). In press. [2] M. K. Jha, A. Kumari, P. K. Choubey, J.-c. Lee, V. Kumar and J. Jeong, Hydrometallurgy, 121-124 (2012) 28-34. [3] P. M. H. Petter, H. M. Veit and A. M. Bernardes, Waste Management, 34 (2014) 475-482. [4] M. Kaya, Waste Management, 57(2016) 64-90. [5] M. F. Bari, M. S. Hossain, I. M. Mujtaba, S. B. Jamaluddin and K. Hussin, Hydrometallurgy, 95 (2009) 308-315. [6] M. S. Hossain, M. F. Bari, S. B. Jamaludin, K. Hussin and M. O. A. Kadir, Korean Journal of Chemical Engineering, 29 (2012) 668-675. [7] S. v. Manivannan, Environmental Innovation and Societal Transitions, 21 (2016) 69-79. [8] A. Tuncuk, V. Stazi, A. Akcil, E. Y. Yazici and H. Deveci, Minerals Engineering, 25 (2012) 28-37. [9] C. Hagelüken, IEEE International Symposium on Electronics & the Environment, 8–11 May, San Francisco, (2006), pp. 218–233. [10] M. Chen, J. Huang, O. A. Ogunseitan, N. Zhu and Y.-m. Wang, Waste Management, 41 (2015) 142-147.