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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\u2013) 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\u2022\u2013) and hydroxyl (\u2022OH) 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.<\/jats:p>","DOI":"10.1021\/acs.est.6c06510","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T20:01:28Z","timestamp":1790884888000},"page":"29138-29148","source":"Crossref","is-referenced-by-count":0,"title":["Photovoltaic-Coupled\nElectrocatalysis System for On-Site\nPersulfate Generation and Sustainable Lithium Extraction"],"prefix":"10.1021","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0241-6707","authenticated-orcid":true,"given":"Xiang-Yang","family":"Lou","sequence":"first","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]},{"name":"Shenzhen University of Information Technology , , ,","place":["Shenzhen, China, 518172"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuezhen","family":"Feng","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Songhe","family":"Yang","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaosong","family":"Gu","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongxin","family":"Chen","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shan","family":"Liu","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxin","family":"Liang","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yangzi","family":"Shangguan","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingsong","family":"Jiang","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhijun","family":"Dong","sequence":"additional","affiliation":[{"name":"Shenzhen University of Information Technology , , ,","place":["Shenzhen, China, 518172"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4053-7147","authenticated-orcid":true,"given":"Hong","family":"Chen","sequence":"additional","affiliation":[{"name":"Southern University of Science and Technology , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,1]]},"reference":[{"issue":"12","key":"2026101310165036300_cit1","doi-asserted-by":"publisher","first-page":"2200099","DOI":"10.1002\/gch2.202200099","article-title":"Current Challenges in Efficient Lithium-Ion Batteries\u2019 Recycling:\nA Perspective","volume":"6","author":"Yu","year":"2022","journal-title":"Global Challenges"},{"issue":"11","key":"2026101310165036300_cit2","doi-asserted-by":"publisher","first-page":"2622","DOI":"10.1016\/j.joule.2019.09.014","article-title":"Recycling\nEnd-of-Life Electric Vehicle Lithium-Ion Batteries","volume":"3","author":"Chen","year":"2019","journal-title":"Joule"},{"key":"2026101310165036300_cit3","doi-asserted-by":"publisher","first-page":"100169","DOI":"10.1016\/j.etran.2022.100169","article-title":"Critical Review of Life Cycle Assessment\nof Lithium-Ion Batteries for Electric Vehicles: A Lifespan Perspective","volume":"12","author":"Lai","year":"2022","journal-title":"eTransportation"},{"issue":"1","key":"2026101310165036300_cit4","doi-asserted-by":"publisher","first-page":"4648","DOI":"10.1038\/s41467-023-40369-9","article-title":"Reaction-Passivation Mechanism Driven\nMaterials Separation for Recycling of Spent Lithium-Ion Batteries","volume":"14","author":"Chen","year":"2023","journal-title":"Nat. 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