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The large-scale implementations of lithium iron phosphate (LFP) batteries for energy storage systems have been gaining attention around the world due to their quality of high technological maturity and flexible configuration. Unfortunately, the exponential production of LFP batteries is accompanied by an annual accumulation of spent batteries and a premature consumption of the lithium resource. Recycling souring critical battery materials such as Li₂CO₃ is essential to reduce the supply chain risk and achieve net carbon neutrality goals. During the recovery of Li₂CO₃, impurity removal is the most crucial step in the hydrometallurgy process of spent LiFePO₄, which determines the purity of Li₂CO₃. By investigating and comparing the results of impurity elimination from the purified Li⁺-containing liquids with strong and weak alkalis under identical pH conditions, respectively, a strategy based on an alkali mixture has been proposed. The purified Li⁺-containing liquid was, thereafter, concentrated and sodium carbonate was added in order to precipitate Li₂CO₃. As a result, a high purity Li₂CO₃ (99.51%) of battery grade was obtained. LiFePO₄ prepared with the recovered Li₂CO₃ and FePO₄ as raw materials also displayed a comparative high capacity and stable cycle performance to the commercial product and further verified the electrochemical activity of the recovered materials.