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Photovoltaic-Coupled Electrocatalysis System for On-Site Persulfate Generation and Sustainable Lithium Extraction
Xiang-Yang Lou1,2, Xuezhen Feng1, Songhe Yang1
1State Key Laboratory of Soil Pollution Control and Safety, MEE Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen518055, China.
Abstract:
The ever-increasing global demand for lithium-based energy storage requires green, economically viable strategies for the recovery of critical metals. Here, we report a photovoltaic-coupled electrocatalytic (PV-EC) system for efficient lithium recovery from spent LiFePO4 (LFP) cathodes by on-site electrochemical generation of persulfate (S2O82-) at a Ti/SnO2/PbO2 anode. Under optimal conditions, we achieved 100% lithium leaching efficiency in the two-electrode system in the laboratory. Mechanistic analysis reveals a tripartite, synergistic oxidation pathway: the electrocatalytically generated sulfate (SO4•-) and hydroxyl (•OH) radicals work in concert with direct electrode oxidation to facilitate a rapid LiFePO4-to-FePO4 phase transition, thereby ensuring preferential lithium leaching. Furthermore, we construct a PV-driven PV-EC system under outdoor conditions, and the system achieves a lithium leaching efficiency of 99.34% in 160 min with minimal iron dissolution, yielding recovered Li3PO4 product with a purity of 95.64%. A techno-economic assessment based on experimental conditions indicates a potential net profit of 1219.66 USD per ton of processed LFP material. The PV-EC system developed here for on-site persulfate generation and lithium leaching offers a feasible, green-chemistry approach for effective critical metal recovery from spent LFP cathodes, with potential extension to other urban mines and mineral tailings.
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