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Upcycling SLCO into high-voltage lithium cobalt oxide (LCO) potentiates its high-value-added utilization; however, single-functional lithium sources in existing regeneration processes only achieve basic lithium compensation and fail to simultaneously address the bottlenecks of bulk structural degradation and uncontrolled interfacial side reactions under 4.6 V high-voltage cycling, which hinders the stable upcycling of SLCO into high-voltage LCO. Herein, a bulk-interface and dual-domain stabilization strategy is proposed via one-step solid-state sintering with lithium cysteinate (Li-Cys). The preferential cleavage of Li\u2013S bonds in Li-Cys first enables targeted lithium compensation for spent LiCoO2, followed by the introduction of NaOH to provide a mild alkaline environment, thereby simultaneously achieving Na\/S co-doping in the bulk and the in situ construction of a Li2SO4\/LiNxOy coating at the interface. Na+ stabilized the layered structure as an interlayer pillar, S enhanced the lattice oxygen stability, and the coating suppressed interfacial side reactions, jointly improving the structural stability and ion transport kinetics. The regenerated NS-RLCO cathode delivered an initial capacity of 205 mAh\/g at 0.1C, 91.9% capacity retention after 100 cycles at 1C, and 158.9 mAh\/g reversible capacity at 3C. Economic and life-cycle analyses confirmed its superior cost and environmental benefits over traditional recycling processes, providing a novel route for environmentally friendly, high-value regeneration of spent LCO.<\/jats:p>","DOI":"10.1021\/acsami.6c08983","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T03:12:42Z","timestamp":1787627562000},"page":"46235-46246","source":"Crossref","is-referenced-by-count":0,"title":["Bulk-Interface and Dual-Domain Stabilization of Spent LiCoO2 Using Multifunctional Lithium Cysteinate Enables High-Voltage Regeneration of Layered Cathodes"],"prefix":"10.1021","volume":"18","author":[{"given":"Tiansheng","family":"Wang","sequence":"first","affiliation":[{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixin","family":"Lin","sequence":"additional","affiliation":[{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zeqiang","family":"Zheng","sequence":"additional","affiliation":[{"name":"Shenzhen Shinehigh Innovation Technology Ltd. , Taoyuan Street , Nanshan District, ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chaochao","family":"Gao","sequence":"additional","affiliation":[{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5220-3238","authenticated-orcid":true,"given":"Jie","family":"Xu","sequence":"additional","affiliation":[{"name":"Harbin Institute of Technology , , ,","place":["Harbin, China, 150080"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5960-1247","authenticated-orcid":true,"given":"Wen","family":"Yu","sequence":"additional","affiliation":[{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2377-9796","authenticated-orcid":true,"given":"Jiaheng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Harbin Institute of Technology (Shenzhen) , , ,","place":["Shenzhen, China, 518055"]},{"name":"Shenzhen Shinehigh Innovation Technology Ltd. , Taoyuan Street , Nanshan District, ,","place":["Shenzhen, China, 518055"]},{"name":"University of Idaho , , , ,","place":["Moscow, Idaho, United States, 83844-2343"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,22]]},"reference":[{"issue":"1","key":"2026101216064515300_cit1","doi-asserted-by":"publisher","first-page":"33","DOI":"10.1007\/s41918-024-00231-y","article-title":"A Deep Dive into Spent Lithium-Ion Batteries: from Degradation Diagnostics to Sustainable Material Recovery","volume":"7","author":"Bai","year":"2024","journal-title":"Electrochem. 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