Department of Chemistry

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Author: search.filters.author.Rao, AnishSubject: search.filters.subject.Electrostatics

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    Revealing the role of electrostatics in gold-nanoparticle-catalyzed reduction of charged substrates
    (ACS, 2017-09) Rao, Anish
    The potency of electrostatic effects arising from nanoparticle (NP) surface in Au-NP-catalyzed reduction of charged substrates are presented. The electrostatic potential around Au NPs is controlled by varying the nature of ligands and ionic strength of the medium. Favorable interactions arising from the attraction between oppositely charged Au NP and substrates results in the channeling of substrates to the NP surface, which in turn enhances the catalytic reduction. The positively charged ([+]) Au NP outperformed other NP systems despite having comparable or even lower surface area for adsorption, proving the exclusivity of electrostatics in catalysis. At least an order of magnitude higher concentration of negatively charged ([−]) Au NP is required to compete with the catalytic activity of [+] Au NP.
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    Electrostatically driven multielectron transfer for the photocatalytic regeneration of nicotinamide cofactor
    (ACS, 2020) Rao, Anish
    Developing generic strategies that are capable of driving multielectron processes are essential to realize important photocatalytic conversions. Here, we present the idea of introducing favorable catalyst–reactant interaction in achieving efficient photocatalytic regeneration of nicotinamide (NADH) cofactor by gold nanoparticles (AuNPs). The electrostatic attraction emanating from the ligands on the surface of NP increases the channeling and local concentration of NAD+ reactants around AuNP photocatalysts, thereby enhancing the probability of the electron transfer process. Detailed kinetics- and intensity-dependent studies confirm the involvement of multiple electron transfer from the AuNP photocatalyst to the NAD+ reactant. The photocatalytic performances of AuNPs presented here are comparable to or greater than most of the catalytic systems reported based on plasmonic NP, with the added advantage of being structurally less complex. The use of electrostatics mimics the underlying force involved in various enzyme catalysis, which can serve as a generic approach for other important artificial multielectron photocatalytic reactions as well.