Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater

doi:10.1007/s11705-019-1806-3

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (4) : 639-650 https://doi.org/10.1007/s11705-019-1806-3

RESEARCH ARTICLE

Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater

Chunlong Zhao^1,², Mingming He², Hongbin Cao², Xiaohong Zheng², Wenfang Gao², Yong Sun³, He Zhao², Dalong Liu⁴, Yanling Zhang¹, Zhi Sun²(

)

¹. State Key Laboratory of Advanced Metallurgy, University of Science and Technology Beijing, Beijing 100083, China
². Beijing Engineering Research Center of Process Pollution Control, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
³. University of Nottingham Ningbo China, Ningbo 315100, China
⁴. Henan Bingsheng Biotechnology Company Limited, Kaifeng 475103, China

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Abstract

In the production of lithium-ion batteries (LIBs) and recycling of spent LIBs, a large amount of low-concentration lithium-containing wastewater (LCW) is generated. The recovery of Li from this medium has attracted significant global attention from both the environmental and economic perspectives. To achieve effective Li recycling, the features of impurity removal and the interactions among different ions must be understood. However, it is generally difficult to ensure highly efficient removal of impurity ions while retaining Li in the solution for further recovery. In this study, the removal of typical impurity ions from LCW and the interactions between these species were systematically investigated from the thermodynamic and kinetics aspects. It was found that the main impurities (e.g., Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺) could be efficiently removed with high Li recovery by controlling the ionic strength of the solution. The mechanisms of Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺ removal were investigated to identify the controlling steps and reaction kinetics. It was found that the precipitates are formed by a zero-order reaction, and the activation energies tend to be low with a sequence of fast chemical reactions that reach equilibrium very quickly. Moreover, this study focused on Li loss during removal of the impurities, and the corresponding removal rates of Fe³⁺, Al³⁺, Ca²⁺, and Mg²⁺ were found to be 99.8%, 99.5%, 99%, and 99.7%, respectively. Consequently, high-purity Li₃PO₄ was obtained via one-step precipitation. Thus, this research demonstrates a potential route for the effective recovery of Li from low-concentration LCW and for the appropriate treatment of acidic LCW.

Keywords lithium-containing wastewater lithium phosphate precipitation impurity ion

Corresponding Author(s): Zhi Sun

Just Accepted Date: 05 May 2019 Online First Date: 25 June 2019 Issue Date: 22 May 2020

Cite this article:

Chunlong Zhao,Mingming He,Hongbin Cao, et al. Investigation of solution chemistry to enable efficient lithium recovery from low-concentration lithium-containing wastewater[J]. Front. Chem. Sci. Eng., 2020, 14(4): 639-650.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1806-3
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I4/639

Tab.1 Initial concentration of different ions in the Li-containing wastewater

Fig.1 Schematic diagram of the experimental device

Tab.2 Concentration of different ions after removing Fe and Al

Fig.2 E-pH diagram for the (a) Fe-H₂O and Al-H₂O, (b) Ca-C-H₂O and Mg-H₂O systems, and (c) Li-P-H₂O systems (at 1 atm pressure and 298 K, c(Fe³⁺) = 0.001432 mol?L⁻¹, c(Al³⁺) = 0.0148 mol?L⁻¹, c(Ca²⁺) = 0.0075 mol?L⁻¹, c(Mg²⁺) = 0.0125 mol?L⁻¹, c(Li⁺) = 1 mol?L⁻¹

Fig.3 Effect of ionic strength on the rate of Li⁺ loss

Fig.4 Zero-order control model for kinetics of removal of (a) Fe³⁺, (b) Al³⁺, (c) Ca²⁺, and (d) Mg²⁺ at different temperatures

Tab.3 Kinetics parameters for ion removal—calculated by applying the zero-order chemical reaction model

Fig.5 Arrhenius plot for the removal of (a) Fe³⁺, (b) Al³⁺, (c) Ca²⁺, and (d) Mg²⁺ in the temperature range of 298K–323 K

Fig.6 (a) XRD pattern of residue after removing Fe³⁺ and Al³⁺ (1) and after baking at 600°C for 2 h (2); (b) simultaneous TG/DSC curves for the residue after removing Fe³⁺ and Al³⁺

Fig.7 (a) XRD pattern of the residue after removing Ca²⁺ and Mg²⁺ and (b) curves for simultaneous TG/DSC analysis of residue after removing Ca²⁺ and Mg²⁺

Fig.8 Mechanisms of removing (a) Fe³⁺ and Al³⁺, and (b) Ca²⁺ and Mg²⁺

Tab.4 Mass fraction of metals in precipitated Li₃PO₄

Fig.9 XRD pattern of recycled Li₃PO₄

Fig.10 SEM image of precipitated Li₃PO₄

Tab.5 Global recovery rates of Li in this research

Fig.11 Simplified flow-sheet for recovery Li from low-concentration LCW

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