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The transformation proceeds under mild, transition-metal-free conditions and exhibits pronounced solvent-dependent chemoselectivity, affording selenourea-functionalized benzimidazoles in water and urea analogues in DMSO. The protocol features broad substrate scope, excellent functional group tolerance, and compatibility with both aromatic and aliphatic secondary amines, enabling late-stage functionalization of bioactive molecules. Mechanistic investigations suggest initial formation of selenourea-containing benzimidazoles via cascade cyclization, followed by DMSO\/O2-mediated oxidative deselenization in the presence of base to furnish the urea products. This work provides a concise and versatile strategy for the divergent construction of benzimidazole-based heterocyclic hybrids.<\/jats:p>","DOI":"10.1021\/acs.orglett.6c02761","type":"journal-article","created":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T13:02:22Z","timestamp":1785934942000},"page":"10302-10307","source":"Crossref","is-referenced-by-count":0,"title":["Solvent-Controlled\nDivergent Synthesis of (Seleno)urea-Containing\nBenzimidazoles from 1,2-Diisocyanobenzenes and Secondary Amines"],"prefix":"10.1021","volume":"28","author":[{"given":"Dongping","family":"Xu","sequence":"first","affiliation":[{"name":"Huangshan University , , ,","place":["Huangshan, P. R. China, 245041"]},{"name":"Anhui Normal University , , ,","place":["Wuhu, P. R. China, 241000"]},{"name":"Anhui Medical University , , ,","place":["Hefei, P. R. 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