Advanced Materials Research Vols 807-809 (2013) pp 1262-1265 © (2013) Trans Tech Publications, Switzerland doi:10.4028/www.scientific.net/AMR.807-809.1262 Online: 2013-09-10 Investigation on the extraction of aluminum and iron from fly ash by sodium carbonate fusion method Hongjing Han1, a, Yanguang Chen1, b, Jia Lu1, c, Dandan Yuan1, d, Jun Song1, e, Ying Chen1, f 1 Provincial Key Laboratory of oil & Gas Chemical Technology, College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing, P.R.China a hongjing_han@163.com, bygchen79310@126.com, clu-jia2008@163.com, d yuandandan111@163.com, emsongjun@163.com, fchenying648617@163.com Keywords: Aluminum extraction, fly ash, sodium carbonate fusion method Abstract: In recent years, utilization of fly ash has gained much attention in public and industry, which will help reduce the environmental burden and enhance economic benefit. In the utilizations of fly ash, the most high value-added applications is extraction of metal elements from fly ash. In this paper, the aluminum and iron extraction was investigated by orthogonal experiments. The results show that the optimum extraction condition was reaction temperature 800 oC, reaction time 3 h, the mass ratio of fly ash to Na2CO3 was 1:1.5. Introduction Fly ash is a type of solid waste from thermal power plants, steel mills, etc. It is in abundance in the world. The production of fly ash is about 3.0×109 t at present. With the sustained and rapid development of China's economy, the energy demand increases. A large amount of fly ash emissions not only occupied land, but also polluted water and atmosphere resources, moreover, it is harmful to human health. Fly ash contains many elements can be recycled [1-3], such as silicon, aluminum and iron, which will help reduce the environmental burden and enhance economic benefit. In the recycling of aluminum, iron, silicon from fly ash, the key problem is how to effectively break the Al-Si bond. the aluminum, silicon and other elements can be made full use of [4, 5]. In this paper, a new method of extracting aluminum and iron was discussed. The calcination reaction between fly ash and Na2CO3 in the high temperature was investigated. The calcined samples were leached by acid, the concentration of aluminum ions and iron ions in the leaching solution were analyzed by titration and spectrophotography, respectively. Experimental Experimental materials The main raw material, coal fly ash samples were collected from Heilongjiang Province of China. Table 1 presents the composition analysis of fly ash. The raw fly ash samples were first screened to the size of 150-200 mesh. The unburned carbon (4.5wt%) presented in fly ash were removed by muffle furnace at 800℃ for 2h. The calcined fly ash samples were treated with distilled water to removal soluble substances. The slurry was dried at 80℃. All rights reserved. No part of contents of this paper may be reproduced or transmitted in any form or by any means without the written permission of Trans Tech Publications, www.ttp.net. (ID: 145.94.211.194, TU Delft, Delft, Netherlands-08/05/15,12:15:10) Advanced Materials Research Vols. 807-809 1263 Table 1 Composition of fly ash Composition SiO2 Al2O3 Fe2O3 TiO2 CaO MgO K2O Na2O Content/wt% 51.44 32.4 6.76 1.58 3.53 1.62 0.80 1.87 Sintered test and leaching test Take a certain amount of fly ash with addition of Na2CO3 into muffle furnace at different temperatures ranging from 760-840℃ for 6h, and then cool down to room temperature and obtain the sample for leaching step. Sintered product was grinded and put into a flask with a stirring device. The hydrochloric acid was added to flask, then it was heated by water bath to reaction with continuous stirring at 250 rpm. In order to prevent hydrochloric acid from evaporation, the flask connected with a condensation device. After fully reacted, the upper liquid and solid was separated. The concentration of aluminum ions and iron ions of leaching solution were calculated by the following equation. ε Al = 3+ mAl × 100% ϕ1m flyash (1) ε Fe = mFe × 100% ϕ 2 m flyash (2) 3+ Where, εFe3+, εAl3+ represented the leaching rates of the concentration of aluminum ions and iron ions. φ1, φ2 represented mass ratio of aluminum and iron elements in fly ash. Process flow diagram experiment are shown as follows. Results and discussion XRD characterization Figure 1 shows that the main crystalline phase was mullite cordierite by X ray diffraction analysis. The samples contained both amorphous (mainly SiO2, Al2O3) and crystalline components (mainly quartz and mullite cordierite). Fig.1 X ray diffraction pattern of fly ash sample Orthogonal experiment To obtain the optimal process condition parameters, orthogonal experiment was designed and investigated. The sintering time ,reaction temperature, and the mass ratio of fly ash to Na2CO3 as influencing factors were investigated. The leaching conditions: 80℃, 3mol/L HCl, leaching time 30min and the ratio of solid to liquid 1g:10mL. The leaching of aluminum and iron rate in fly ash were analyzed as the main indexes of orthogonal experiments, the results was shown in Table 2. 1264 X Y Environmental Protection and Resources Exploitation SN T/oC 1 2 3 4 5 6 7 8 9 760 760 760 800 800 800 840 840 840 31.99 42.21 51.11 19.11 55.51 80.35 84.85 29.34 K1 K2 K3 R1 K1 K2 K3 R2 Table 2 The results of orthogonal experiments X (Al3+ leaching rate Y (Fe3+ leaching rate t/h mfly ash/mNa2CO3 /%) /%) 25.40 1 1:1 43.16 24.99 2 1:1.5 57.26 46.70 3 1:2 66.10 40.09 1 1:1.5 57.77 41.38 2 1:2 92.56 54.43 3 1:1 90.72 45.60 1 1:2 75.70 45.15 2 1:1 86.56 52.19 3 1:1.5 92.28 41.66 37.40 39.09 40.27 44.56 47.65 5.47 10.25 58.88 73.48 78.79 69.10 83.03 78.12 24.16 9.018 can determine the impact of various factors on the leaching effect of aluminum and iron ions after the activation of fly ash: Sintering temperature> reaction time > the ratio of fly ash to Na2CO3. It can be seen that the factors on the leaching of aluminum and iron ions of fly ash activated by Na2CO3 are different. the optimal scheme is A3B3C3, however, this scheme is not in our orthogonal experiments. A proof test was done, the condition is as following: sintering time 3h, the sintering temperature 840oC, the ratio fly ash to Na2CO3 1:2 and acid concentration 3mol/L. The leaching ratio of aluminum ion and iron ion was 52.78% and 95.55%. It can be seen from the above table, the leaching ratio of the proof test was similar with the result of the ninth orthogonal test. In consideration with saving raw materials, the scheme A3B3C2 was selected. Extraction without addition of Na2CO3 Fly ash samples without addition of Na2CO3 was also leached by acid directly. Other processing conditions are the same, the results was shown in Fig. 2. The leaching ratio of aluminum ion and iron ion were only 14.02% and 42.3%, far lower than 52.78% and 95.55% in Na2CO3 fusion method. After activation of fly ash under high temperatures with sodium carbonate, Si-Al bond in the fly ash was broken, the aluminum ion and iron ion leaching ratio increased significantly. Advanced Materials Research Vols. 807-809 1265 50 aluminum ion iron ion Removal rate/% 40 30 20 10 0.5 1.0 1.5 2.0 2.5 Time/h Fig.2 Results of extraction of aluminum and iron without addition of Na2CO3 Conclusions The aluminum and iron was extracted from fly ash by using Na2CO3 fusion method, the orthogonal experiment was designed and investigated, the follow conclusion can be obtained: (1) Fly ash was activated by Na2CO3 fusion method. The order of the influencing factors is: sintering temperature> reaction time > the ratio of fly ash to Na2CO3. (2) The optimum processing parameters are sintering temperature 800oC, reaction time 3 h, the mass ratio of fly ash to Na2CO3 was 1:1.5 and hydrochloric acid concentration 3mol/L. Under this condition, the ratio of aluminum and iron ion are 52.78% and 95.55%, respectively. (3) Fly ash without the activated by Na2CO3, the ratio of aluminum ion and iron ion in leaching test is 14.02% and 42.3%, lower than that in Na2CO3 fusion method. Acknowledgements This work was financially supported by National Natural Science Foundation of China (No.51204057), National Postdoctoral Science Foundation of China (No.2012M510918), Science Foundation for Young Scholars of Heilongjiang Province of China (QC2011C034), Foundation for Key Teacher of Universities by Heilongjiang Province of China (1252G007), Project of Science and Technology of Heilongjiang Province of China (No.12521054) and Heilongjiang Postdoctoral Grant (LBH-Z12274). References [1] N. Nayak, C.R. Panda. Aluminum extraction and leaching characteristics of Talcher Thermal Power Station fly ash with sulphuric acid[J]. Fuel, 2010, 89(1): 53-58. [2] C.Y Wu, H.F. Yu, H.F. Zhang. Extraction of aluminum by pressure acid-leaching method from coal fly ash[J]. Transactions of Nonferrous Metals Society of China, 2012, 22(9): 2282-2288. [3] A. Seidel, Y. Zimmels. Mechanism and kinetics of aluminum and iron leaching from coal fly ash by sulfuric acid[J]. Chemical Engineering Science, 1998, 53(22): 3835-3852. [4] A. Shemi, R.N. Mpana, S. Ndlovu, et al. Alternative techniques for extracting alumina from coal fly ash[J]. Minerals Engineering, 2012, 34(1): 30-37. [5] T. Hirajimaa, H.T.B.M. Petrusb, Y. Oosakob, et al. Recovery of cenospheres from coal fly ash using a dry separation process: Separation estimation and potential application[J]. International Journal of Mineral Processing, 2010, 95(1-4): 18-24. Environmental Protection and Resources Exploitation 10.4028/www.scientific.net/AMR.807-809 Investigation on the Extraction of Aluminum and Iron from Fly Ash by Sodium Carbonate Fusion Method 10.4028/www.scientific.net/AMR.807-809.1262 DOI References [1] N. Nayak, C.R. Panda. Aluminum extraction and leaching characteristics of Talcher Thermal Power Station fly ash with sulphuric acid[J]. Fuel, 2010, 89(1): 53-58. http://dx.doi.org/10.1016/j.fuel.2009.07.019 [2] C. Y Wu, H.F. Yu, H.F. Zhang. Extraction of aluminum by pressure acid-leaching method from coal fly ash[J]. Transactions of Nonferrous Metals Society of China, 2012, 22(9): 2282-2288. http://dx.doi.org/10.1016/S1003-6326(11)61461-1 [3] A. Seidel, Y. Zimmels. Mechanism and kinetics of aluminum and iron leaching from coal fly ash by sulfuric acid[J]. Chemical Engineering Science, 1998, 53(22): 3835-3852. http://dx.doi.org/10.1016/S0009-2509(98)00201-2 [4] A. Shemi, R.N. Mpana, S. Ndlovu, et al. Alternative techniques for extracting alumina from coal fly ash[J]. Minerals Engineering, 2012, 34(1): 30-37. http://dx.doi.org/10.1016/j.mineng.2012.04.007