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Received February 10, 2022
Accepted June 12, 2022
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This is an Open-Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/bync/3.0) which permits
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A facile method for efficient synergistic oxidation of Fe2+ in phosphorus-sulfur mixed acid system with a mixture of oxygen and ozone
1Normal College, Shenyang University, Shenyang 110044, China 2School of Metallurgy, Northeastern University, Shenyang 110819, China 3National Engineering Research Center of Green Recycling for Strategic Metal Resources, Chinese Academy of Sciences, Institute of Process Engineering, Beijing 100190, China 4Institute of Innovative Science and Technology, Shenyang University, Shenyang 110044, China
wbolou@163.com
Korean Journal of Chemical Engineering, December 2022, 39(12), 3323-3333(11), 10.1007/s11814-022-1206-0
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Abstract
The recovery of iron phosphate involves the addition of oxidizer to oxidize Fe2+ in the spent LiFePO4 (LFP) material to Fe3+ and the agent commonly used is hydrogen peroxide (H2O2). Nevertheless, H2O2 has disadvantages of high price, easy decomposition and low utilization efficiency. In this manuscript, a facile method is proposed for efficient synergistic oxidation of Fe2+ in spent LFP leachate with a mixture of oxygen and ozone. Specifically, we found by thermodynamic computations that the dominant oxidation groups of ozone during oxidation varied with acidity. The oxidation would produce a large number of iron-phosphate complex groups (Fe3H6(PO4)4 3+, FeH8(PO4)4 - and Fe2HPO4 4+) in the phosphorus-sulfur mixed acid system, leading to a paradoxical pH drop. The optimized conditions for H2O2 oxidation were explored. It was determined experimentally that oxidation by gas mixture and O2 belonged to the firstorder and second-order reactions with activation energies of 28.68 kJ/mol and 34.61 kJ/mol, respectively, which were both controlled by a mixture of chemical reaction and diffusion. The optimized oxidation method was finally determined by evaluating the cost and oxidation rate of the oxidizers. The results in this study offer a promising method for new low-cost and efficient Fe2+ oxidation for industrial production.
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Zhang Y, Sun W, Xu R, Wang L, Tang H, J. Clean Prod., 285, 124905 (2021)
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Murahashi SI, Oda Y, Naota T, Tetrahedron Lett., 33, 7557 (1992)
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Li M, Chen Z, Wang Z, Wen Q, Chemosphere, 217, 223 (2019)
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Cao X, Zhang TA, Liu Y, Zhang W, Li S, Lv G, Han X, Nonferrous Met. Sci. Eng., 11, 1 (2020)
Jiang F, Qiu B, Sun D, Chem. Eng. J., 370, 346 (2001)
Bourgin M, Beck B, Boehler M, Borowska E, Fleiner J, Salhi E, Teichler R, von Gunten U, Siegrist H, McArdell CS, Water Res., 129, 486 (2018)
Jia W, Wang F, Wang M, Wang D, Zheng L, Ding A, Liu B, Liang X, Yu HU, S. N. Water Transfers Water Water Sci. Technol., 17, 113 (2019)
Tao T, Shaoxian S, Jierong Y, Chin. J. Power Sources, 44, 17 (2020)
Wang Y, Lü Y, Wang S, Du H, Chin. J. Process Eng., 21, 877 (2021)
Yang TC, Neely WC, Anal. Chem., 58, 1551 (1986)
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Loegager T, Holcman J, Sehested K, Pedersen T, Inorg. Chem., 31, 3523 (1992)
Schulte P, Bayer A, Kuhn F, Luy T, Volkmer M, Ozone: Sci. Eng., 17, 119 (1995)
Lou WB, Zhang Y, Zhang Y, Zheng SI, Sun P, Wang XJ, Li JZ, Qiao S, Zhang Y, Wenzel M, Weigand JJ, Trans. Nonferrous Met. Soc. China, 31, 817 (2021)
Lou WB, Zhang Y, Zhang Y, Zheng SI, Sun P, Wang XJ, Qiao S, Li JZ, Zhang Y, Liu DY, Wenzel M, Weigand JJ, J. Alloy. Compd., 856, 158148 (2020)
