A green and sustainable strategy toward lithium resources recycling from spent batteries.

Xu, Jing; Jin, Yang; Liu, Kai; Lyu, Nawei; Zhang, Zili; Sun, Bin; Jin, Qianzheng; Lu, Hongfei et al. · Sci Adv · 2022

basic_science · Level V

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Abstract

Recycling lithium from spent batteries is challenging because of problems with poor purity and contamination. Here, we propose a green and sustainable lithium recovery strategy for spent batteries containing LiFePO<sub>4</sub>, LiCoO<sub>2</sub>, and LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub> electrodes. Our proposed configuration of "lithium-rich electrode || LLZTO@LiTFSI+P3HT || LiOH" system achieves double-side and roll-to-roll recycling of lithium-containing electrode without destroying its integrity. The LiTFSI+P3HT-modified LLZTO membrane also solves the H<sup>+</sup>/Li<sup>+</sup> exchange problem and realizes a waterproof protection of bare LLZTO in the aqueous working environment. On the basis of these advantages, our system shows high Li selectivity (97%) and excellent Faradaic efficiency (≥97%), achieving high-purity (99%) LiOH along with the production of H<sub>2</sub>. The Li extraction processes for spent LiFePO<sub>4</sub>, LiNi<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>O<sub>2</sub>, and LiCoO<sub>2</sub> batteries is shown to be economically feasible. Therefore, this study provides a previously unexplored technology with low energy consumption as well as high economic and environmental benefits to realize sustainable lithium recycling from spent batteries.