000124047 001__ 124047 000124047 005__ 20230914083808.0 000124047 0247_ $$2doi$$a10.1021/jacsau.1c00477 000124047 0248_ $$2sideral$$a132675 000124047 037__ $$aART-2022-132675 000124047 041__ $$aeng 000124047 100__ $$aRodenes, Miriam 000124047 245__ $$aMolecularly engineering Defective Basal Planes in Molybdenum Sulfide for the direct synthesis of Benzimidazoles by Reductive Coupling of Dinitroarenes with Aldehydes 000124047 260__ $$c2022 000124047 5060_ $$aAccess copy available to the general public$$fUnrestricted 000124047 5203_ $$aDeveloping more sustainable catalytic processes for preparing N-heterocyclic compounds in a less costly, compact, and greener manner from cheap and readily available reagents is highly desirable in modern synthetic chemistry. Herein, we report a straightforward synthesis of benzimidazoles by reductive coupling of o-dinitroarenes with aldehydes in the presence of molecular hydrogen. An innovative molecular cluster-based synthetic strategy that employs Mo3S4 complexes as precursors have been used to engineer a sulfur-deficient molybdenum disulfide (MoS2)-type material displaying structural defects on both the naturally occurring edge positions and along the typically inactive basal planes. By applying this catalyst, a broad range of functionalized 2-substituted benzimidazoles, including bioactive compounds, can be selectively synthesized by such a direct hydrogenative coupling protocol even in the presence of hydrogenation-sensitive functional groups, such as double and triple carbon–carbon bonds, nitrile and ester groups, and halogens as well as diverse types of heteroarenes. 000124047 536__ $$9info:eu-repo/grantAgreement/ES/DGA-FEDER/E31-17R$$9info:eu-repo/grantAgreement/ES/MICINN-AEI-FEDER/PID2019-105881RB-I00 000124047 540__ $$9info:eu-repo/semantics/openAccess$$aby-nc-nd$$uhttp://creativecommons.org/licenses/by-nc-nd/3.0/es/ 000124047 594__ $$a5.3$$b2022 000124047 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/publishedVersion 000124047 700__ $$aGonell, Francisco 000124047 700__ $$0(orcid)0000-0001-9193-3874$$aMartín, Santiago$$uUniversidad de Zaragoza 000124047 700__ $$aCorma, Avelino 000124047 700__ $$aSorribes, Iván 000124047 7102_ $$12012$$2755$$aUniversidad de Zaragoza$$bDpto. Química Física$$cÁrea Química Física 000124047 773__ $$g2, 3 (2022), 601-612$$tJACS Au$$x2691-3704 000124047 8564_ $$s4164729$$uhttps://zaguan.unizar.es/record/124047/files/texto_completo.pdf$$yVersión publicada 000124047 8564_ $$s3239624$$uhttps://zaguan.unizar.es/record/124047/files/texto_completo.jpg?subformat=icon$$xicon$$yVersión publicada 000124047 909CO $$ooai:zaguan.unizar.es:124047$$particulos$$pdriver 000124047 951__ $$a2023-09-13-15:27:29 000124047 980__ $$aARTICLE