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Here, by developing a bifunctional single-atom cobalt catalyst supported on hierarchical ordered porous carbon matrix (Co\u2013N4\/HPC), it enables hydroxyaminomethylation of nonactivated terminal alkenes with nitroarenes and formaldehyde using HCOOH reductant. This difunctionalization reaction features operational simplicity, high atom\/step economy, broad substrate scope, excellent functionality tolerance, high selectivity, and catalyst reusability, offering a practical platform for the general synthesis of \u03b3-arylamino alcohols from bulk chemicals. Notably, the Co\u2013N4 sites mediate mild reduction, while the mesoporous N-doped carbon support enriches formaldehyde via physical adsorption, facilitating the capture of hydroxylamines formed in situ from nitroarene reduction. Subsequent 1,3-dipolar cycloaddition of the resulting nitrones with alkenes, followed by reduction of the cycloadducts, delivers the desired products. The concept of exploiting metal\u2013support synergy for mild reduction and efficient intermediate conversion will open a door to the further development of useful tandem reactions through rational catalyst design.<\/jats:p>","DOI":"10.1021\/jacs.6c11412","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T19:36:49Z","timestamp":1784662609000},"page":"32816-32826","source":"Crossref","is-referenced-by-count":2,"title":["General Synthesis of\n\u03b3-Arylamino Alcohols\nvia Difunctionalization of Terminal Alkenes Using a Supported Cobalt\nSingle-Atom Catalyst"],"prefix":"10.1021","volume":"148","author":[{"given":"Wei","family":"Liu","sequence":"first","affiliation":[{"name":"South China University of Technology , , ,","place":["Guangzhou, China, 510641"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9060-848X","authenticated-orcid":true,"given":"Mingkai","family":"Liu","sequence":"additional","affiliation":[{"name":"Anhui University of Technology , , , ,","place":["Ma\u2019anshan, Anhui, P. 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