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Here, we present a new type of catalyst model\u2014phase\u2010engineered quantum\u2010monolayer catalyst, as a complementary catalyst architecture that offers high\u2010density accessible atoms and enables versatile phase\/interphase engineering for catalysis. As a prototype (in our 13\u2010type quantum monolayer library), our fabricated MoS\n                    <jats:sub>2<\/jats:sub>\n                    quantum\u2010monolayer catalysts are one molecule\u2010layer thick (\u223c0.8\u00a0nm), quantum\u2010sized (&lt; 6\u00a0nm in the lateral size), and phase controllable (switchable freely among metallic 1T, semiconducting 2H, and hybrid phase of metallic\u2010semiconducting 1T\u20102H). They can be synthesized on a large scale (experimentally demonstrated at a 20\u00a0g scale) with a high quantum\u2010monolayer yield (&gt;99%) and product recovery ratio (&gt;95%); can be stored independently and stably (at 4\u00b0C or in an inert atmosphere) for more than 6 months; can be easily processed into customized structures by solution deposition technologies; and have the potential to be used as a catalyst or co\u2010catalyst for photo\u2010, electro\u2010, and thermo\u2010chemical conversions. We demonstrate their potential for photochemical H\n                    <jats:sub>2<\/jats:sub>\n                    , syngas, and NH\n                    <jats:sub>3<\/jats:sub>\n                    production with high performance and stability.\n                  <\/jats:p>","DOI":"10.1002\/adma.75247","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T09:47:22Z","timestamp":1791452842000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Phase\u2010Engineered MoS\n                    <sub>2<\/sub>\n                    Quantum Monolayer Catalysts"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9410-8439","authenticated-orcid":false,"given":"Ruijie","family":"Yang","sequence":"first","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-5670-2608","authenticated-orcid":false,"given":"Yingying","family":"Fan","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lillian","family":"Pernitsky","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-6650-5771","authenticated-orcid":false,"given":"Mojtaba Ebrahimian","family":"Mashhadi","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-1301-709X","authenticated-orcid":false,"given":"Ningxin","family":"Chen","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9349-9821","authenticated-orcid":false,"given":"Md. Mehadi","family":"Hassan","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-1318-8175","authenticated-orcid":false,"given":"Zheng","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical and Petroleum Engineering University of Calgary  Calgary Alberta Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-6280-3097","authenticated-orcid":false,"given":"Heng","family":"Zhao","sequence":"additional","affiliation":[{"name":"College of Engineering Eastern Institute of Technology  Ningbo Zhejiang P. R. 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