Ag-S Type Quantum Dots versus Superatom Nanocatalyst: A Single Sulfur Atom Modulated Decarboxylative Radical Cascade Reaction

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dc.contributor.authorMeena, Sangeeta
dc.contributor.authorDastider, Saptarshi G.
dc.contributor.authorNishad, Chandra Shekhar
dc.contributor.authorJangid, Dilip Kumar
dc.contributor.authorKumar, Pankaj
dc.contributor.authorKhirid, Samreet
dc.contributor.authorBose, Shubhankar Kumar
dc.contributor.authorMondal, Krishnakanta
dc.contributor.authorBanerjee, Biplab
dc.contributor.authorDhayal, Rajendra S.
dc.date.accessioned2024-01-21T10:33:07Z
dc.date.accessioned2024-08-13T11:16:20Z
dc.date.available2024-01-21T10:33:07Z
dc.date.available2024-08-13T11:16:20Z
dc.date.issued2023-04-06T00:00:00
dc.description.abstractThe preparation of high-nuclearity silver nanoclusters in quantitative yield remains exclusive and their potential applications in the catalysis of organic reactions are still undeveloped. Here, we have synthesized a quantum dot (QD)-based catalyst, [Ag62S13(SBut)32](PF6)4 (denoted as Ag62S12-S) in excellent yield that enables the direct synthesis of pharmaceutically precious 3,4-dihydroquinolinone in 92% via a decarboxylative radical cascade reaction of cinnamamide with ?-oxocarboxylic acid under mild reaction conditions. In comparison, a superatom [Ag62S12(SBut)32](PF6)2 (denoted as Ag62S12) with identical surface anatomy and size, but without a central S2- atom in the core, gives an improved yield (95%) in a short time and exhibits higher reactivity. Multiple characterization techniques (single-crystal X-ray diffraction, nuclear magnetic resonance (1H and 31P), electrospray ionization mass spectrometry, energy dispersive X-ray spectroscopy, Brunauer-Emmett-Teller (BET), Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and thermogravimetric analysis) confirm the formation of Ag62S12-S. The BET results expose the total active surface area in supporting a single e- transfer reaction mechanism. Density functional theory reveals that leaving the central S atom of Ag62S12-S leads to higher charge transfer from Ag62S12 to the reactant, accelerates the decarboxylation process, and correlates the catalytic properties with the structure of the nanocatalyst. � 2023 American Chemical Society.en_US
dc.identifier.doi10.1021/acs.inorgchem.3c00070
dc.identifier.issn201669
dc.identifier.urihttp://10.2.3.109/handle/32116/3271
dc.identifier.urlhttps://pubs.acs.org/doi/10.1021/acs.inorgchem.3c00070
dc.language.isoen_USen_US
dc.publisherAmerican Chemical Societyen_US
dc.subjectAtomsen_US
dc.subjectCarboxylationen_US
dc.subjectCrystal atomic structureen_US
dc.subjectDensity functional theoryen_US
dc.subjectElectrodepositionen_US
dc.subjectElectrospray ionizationen_US
dc.subjectEnergy dispersive spectroscopyen_US
dc.subjectFourier transform infrared spectroscopyen_US
dc.subjectHigh resolution transmission electron microscopyen_US
dc.subjectLigandsen_US
dc.subjectMass spectrometryen_US
dc.subjectNanocatalystsen_US
dc.subjectNanocrystalsen_US
dc.subjectNuclear magnetic resonance spectroscopyen_US
dc.subjectSilver compoundsen_US
dc.subjectSingle crystalsen_US
dc.subjectSulfuren_US
dc.subjectThermogravimetric analysisen_US
dc.subjectX ray photoelectron spectroscopyen_US
dc.subjectBrunauer emmett tellersen_US
dc.subjectNano-catalysten_US
dc.subjectNuclearityen_US
dc.subjectOrganic reactionen_US
dc.subjectQuantitative yieldsen_US
dc.subjectRadical cascade reactionsen_US
dc.subjectSilver nanoclustersen_US
dc.subjectSulphur atomsen_US
dc.subjectSuperatomsen_US
dc.subjectSynthesiseden_US
dc.subjectSemiconductor quantum dotsen_US
dc.titleAg-S Type Quantum Dots versus Superatom Nanocatalyst: A Single Sulfur Atom Modulated Decarboxylative Radical Cascade Reactionen_US
dc.title.journalInorganic Chemistryen_US
dc.typeArticleen_US
dc.type.accesstypeClosed Accessen_US

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