000130221 001__ 130221
000130221 005__ 20241125101152.0
000130221 0247_ $$2doi$$a10.1021/acssuschemeng.3c01489
000130221 0248_ $$2sideral$$a135314
000130221 037__ $$aART-2023-135314
000130221 041__ $$aeng
000130221 100__ $$aRodenes, Miriam
000130221 245__ $$aMultifunctional Catalysis of Nanosheet Defective Molybdenum Sulfide Basal Planes for Tandem Reactions Involving Alcohols and Molecular Hydrogen
000130221 260__ $$c2023
000130221 5060_ $$aAccess copy available to the general public$$fUnrestricted
000130221 5203_ $$aEstablishing tandem catalytic synthetic strategies based on the use of readily available, stable, and renewable feedstocks is of great significant for the sustainable advancement of chemical-related industries. The key to success largely relies on applying efficient multifunctional catalysts that allow carrying out one-pot single-step synthesis. In this work, we have demonstrated that defect-engineered basal planes of a molybdenum sulfide nanomaterial ({Mo3S4}n) offer a multifunctional catalytic platform for chemical process intensification. By applying this catalyst, besides borrowing hydrogen-type processes, herein exemplified for the thioetherification of alcohols, we have also disclosed novel and rare coupling reactions requiring hydrogen activation and alcohol dehydrogenation processes in a one-pot fashion. More specifically, oxidized nucleophiles, such as o-dinitroarenes and dinitrophenyl disulfides, are reacted with alcohols in the presence of H2 to yield respectively benzimidazoles and benzothiazoles. The uncommon catalytic reactivity of {Mo3S4}n arises from the presence of coordinatively unsaturated molybdenum and sulfide species, which work as Lewis acid and Lewis basic sites, respectively. As suggested by in situ infrared (IR) spectroscopy investigations, the alcohol dehydrogenation involves the participation of both types of active sites while the H2 dissociation takes place on coordinatively unsaturated sulfide species.
000130221 540__ $$9info:eu-repo/semantics/openAccess$$aAll rights reserved$$uhttp://www.europeana.eu/rights/rr-f/
000130221 590__ $$a7.1$$b2023
000130221 592__ $$a1.664$$b2023
000130221 591__ $$aENGINEERING, CHEMICAL$$b21 / 170 = 0.124$$c2023$$dQ1$$eT1
000130221 591__ $$aGREEN & SUSTAINABLE SCIENCE & TECHNOLOGY$$b21 / 91 = 0.231$$c2023$$dQ1$$eT1
000130221 591__ $$aCHEMISTRY, MULTIDISCIPLINARY$$b43 / 231 = 0.186$$c2023$$dQ1$$eT1
000130221 593__ $$aEnvironmental Chemistry$$c2023$$dQ1
000130221 593__ $$aRenewable Energy, Sustainability and the Environment$$c2023$$dQ1
000130221 593__ $$aChemistry (miscellaneous)$$c2023$$dQ1
000130221 593__ $$aChemical Engineering (miscellaneous)$$c2023$$dQ1
000130221 594__ $$a13.8$$b2023
000130221 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/acceptedVersion
000130221 700__ $$aDhaeyere, Frederic
000130221 700__ $$0(orcid)0000-0001-9193-3874$$aMartín, Santiago$$uUniversidad de Zaragoza
000130221 700__ $$aConcepción, Patricia
000130221 700__ $$aCorma, Avelino
000130221 700__ $$aSorribes, Iván
000130221 7102_ $$12012$$2755$$aUniversidad de Zaragoza$$bDpto. Química Física$$cÁrea Química Física
000130221 773__ $$g11, 33 (2023), 12265-12279$$pACS sustain. chem. & eng.$$tACS Sustainable Chemistry and Engineering$$x2168-0485
000130221 8564_ $$s1715375$$uhttps://zaguan.unizar.es/record/130221/files/texto_completo.pdf$$yPostprint$$zinfo:eu-repo/semantics/openAccess
000130221 8564_ $$s1139240$$uhttps://zaguan.unizar.es/record/130221/files/texto_completo.jpg?subformat=icon$$xicon$$yPostprint$$zinfo:eu-repo/semantics/openAccess
000130221 909CO $$ooai:zaguan.unizar.es:130221$$particulos$$pdriver
000130221 951__ $$a2024-11-22-12:07:38
000130221 980__ $$aARTICLE