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Here, we utilized a cryogenic engineering strategy to \u201cfreeze\u201d the vulnerable \u03b3-Mo2N surface, coupling with atomically dispersed redox-active Ce1Ox as a dynamic promoter on Pt-\u03b3-Mo2N interfaces. Unlike conventional inert shields that often fail to promote catalytic efficiency, the redox-active Ce1Ox upgraded surface reaction kinetics via electronic modification, meanwhile avoiding irreversible deep oxidation of \u03b3-Mo2N induced by scavenging excessive dissociated *O through reversible redox cycles. We show that integrating a porous, low-temperature passivated Mo2N surface with redox-active Ce1Ox sites dynamically protects against oxidation via reversible Ce3+\/Ce4+ cycling while electronically modulating adjacent Pt to enhance CO adsorption and H2O dissociation, thereby achieving both superior activity and exceptional durability in low-temperature hydrogen production. Consequently, the optimized 1Pt-Ce1Ox\/Mo2N-194 K catalyst achieves a record-high hydrogen production turnover number of 22,500,000 molH2\/molPt alongside outstanding stability exceeding 1500 h in methanol steam reforming. This synergistic approach, merging cryogenic treatment with redox-active shielding, provides a promising paradigm to simultaneously achieve potent catalytic activation and robust structural protection in highly reactive yet inherently vulnerable nanostructures.<\/jats:p>","DOI":"10.1021\/jacs.6c11342","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T22:26:33Z","timestamp":1788215193000},"page":"38244-38255","source":"Crossref","is-referenced-by-count":0,"title":["Pt\/Mo2N\nCatalyst Enabled by Redox Single-Site\nCeO\n                    <i>x<\/i>\n                    for Methanol Steam Reforming"],"prefix":"10.1021","volume":"148","author":[{"given":"Ming","family":"Zhang","sequence":"first","affiliation":[{"name":"Shandong University , , ,","place":["Jinan, China, 250100"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zirui","family":"Gao","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100874"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7215-8307","authenticated-orcid":true,"given":"Jin-Cheng","family":"Liu","sequence":"additional","affiliation":[{"name":"Nankai University , , ,","place":["Tianjin, China, 300350"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8379-0789","authenticated-orcid":true,"given":"Xin-Pu","family":"Fu","sequence":"additional","affiliation":[{"name":"Shandong University , , ,","place":["Jinan, China, 250100"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4471-2152","authenticated-orcid":true,"given":"Wei-Wei","family":"Wang","sequence":"additional","affiliation":[{"name":"Shandong University , , ,","place":["Jinan, China, 250100"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao-Xin","family":"Liu","sequence":"additional","affiliation":[{"name":"University College London , , Roberts Building, Torrington Place , ,","place":["London, U.K., WC1E 7JE"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7713-4398","authenticated-orcid":true,"given":"Mi","family":"Peng","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100874"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wu","family":"Zhou","sequence":"additional","affiliation":[{"name":"University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2475-606X","authenticated-orcid":true,"given":"Feng Ryan","family":"Wang","sequence":"additional","affiliation":[{"name":"University College London , , Roberts Building, Torrington Place , ,","place":["London, U.K., WC1E 7JE"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3341-2998","authenticated-orcid":true,"given":"Ding","family":"Ma","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100874"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4254-5100","authenticated-orcid":true,"given":"Chun-Jiang","family":"Jia","sequence":"additional","affiliation":[{"name":"Shandong University , , ,","place":["Jinan, China, 250100"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0581-2951","authenticated-orcid":true,"given":"Chun-Hua","family":"Yan","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100874"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,25]]},"reference":[{"key":"2026090910075088400_cit1","doi-asserted-by":"publisher","first-page":"547","DOI":"10.1126\/science.181.4099.547","article-title":"Platinum-like\nbehavior of tungsten carbide in surface\ncatalysis","volume":"181","author":"Levy","year":"1973","journal-title":"Science"},{"key":"2026090910075088400_cit2","doi-asserted-by":"publisher","first-page":"588","DOI":"10.1038\/s41565-026-02135-y","article-title":"Single atoms\nof indium on hafnia enable superior CO2-based methanol\nsynthesis","volume":"21","author":"Chiang","year":"2026","journal-title":"Nat. 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