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Vertically aligned MoS2 nanosheets are conformally capped with an amorphous, oxygen-vacancy-rich TiO2 skin. The electrode retains 507 mAh g\u20131 with \u223c100% Coulombic efficiency after 500 cycles at 2 A g\u20131 and delivers 1135 mAh g\u20131 even at 20 A g\u20131. XPS\/UPS quantifies high-density oxygen vacancies (Ovs) in TiO2, while DFT reveals these vacancies lower Li+ adsorption energy to \u22124.003 eV and drive electron accumulation into MoS2. EIS verifies a charge-transfer resistance of only 22.4 \u03a9, and CV confirms pseudocapacitive-dominated kinetics. DOS\/band-alignment analysis substantiates that Ovs generate a built-in electric field pointing from TiO2 to MoS2, which promotes interfacial charge redistribution and accelerates Li+ adsorption and diffusion. These atomistic insights into the interfacial electronic structure modulation highlight an industrially compatible interface-engineering route for fast-charging lithium-ion anodes.<\/jats:p>","DOI":"10.1021\/acsomega.6c04090","type":"journal-article","created":{"date-parts":[[2026,9,8]],"date-time":"2026-09-08T18:02:22Z","timestamp":1788890542000},"page":"55422-55436","source":"Crossref","is-referenced-by-count":0,"title":["Binder-Free MoS2@TiO2 Heterojunction\nby In-Situ Magnetron Sputtering: Interfacial Defect Engineering for\nFast-Charging Anodes"],"prefix":"10.1021","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-8396-9449","authenticated-orcid":true,"given":"Yu","family":"Zhang","sequence":"first","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu","family":"Zeng","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nan","family":"Jin","sequence":"additional","affiliation":[{"name":"China State Grid Hebei Provincial Electric Power Co., LTD. , , ,","place":["Shijiazhuang, China, 050070"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingbo","family":"Kang","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peiyi","family":"Tong","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zening","family":"Li","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5843-8425","authenticated-orcid":true,"given":"Linxia","family":"Wang","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lei","family":"Liu","sequence":"additional","affiliation":[{"name":"Hebei University , , ,","place":["Baoding, China, 071002"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,8]]},"reference":[{"key":"2026092210581041100_cit1","unstructured":"Whittingham, M. 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