Department Of Chemistry

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Author: search.filters.author.Sen, TapasiSubject: search.filters.subject.Electrocatalysts

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    DNA Origami-Templated Bimetallic Core-Shell Nanostructures for Enhanced Oxygen Evolution Reaction
    (American Chemical Society, 2022-04-15T00:00:00) Kaur, Gagandeep; Biswas, Rathindranath; Haldar, Krishna Kanta; Sen, Tapasi
    Hydrogen generation through electrocatalytic water splitting offers promising technology for sustainable and clean energy production as an alternative to conventional energy sources. The development of highly active electrocatalysts is of immense interest for improving the efficiency of gas evolution, which is strongly hindered due to the sluggish kinetics of oxygen evolution reaction (OER). Herein, we present the design of Ag-coated Au nanostar (core-shell-type Au@Ag nanostar) monomer structures assembled on rectangular DNA origami and study their electrocatalytic activities through OER, which remains unexplored. Our designed DNA origami-templated bimetallic nanostar catalyst showed excellent OER activity and high stability without using any external binder and exhibited a current density of 10 mA cm-2at a low overpotential of 266 mV, which was smaller than those of ss-DNA-functionalized Au@Ag nanostars and DNA origami-templated pure Au nanostars. Our results reveal that DNA origami-assembled core-shell Au@Ag nanostars show better electrocatalytic performance as compared to pure-core Au nanostars immobilized on DNA origami, owing to the presence of a highly conductive Ag layer. Such controlled assembly of bimetallic nanostructures on a DNA origami template can provide additional electrochemical surface area and a higher density of active sites resulting in enhanced electrocatalysis. � 2022 American Chemical Society. All rights reserved.
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    Interfacial Engineering of CuCo2S4/g-C3N4Hybrid Nanorods for Efficient Oxygen Evolution Reaction
    (American Chemical Society, 2021-07-29T00:00:00) Biswas, Rathindranath; Thakur, Pooja; Kaur, Gagandeep; Som, Shubham; Saha, Monochura; Jhajhria, Vandna; Singh, Harjinder; Ahmed, Imtiaz; Banerjee, Biplab; Chopra, Deepak; Sen, Tapasi; Haldar, Krishna Kanta
    Altering the morphology of electrochemically active nanostructured materials could fundamentally influence their subsequent catalytic as well as oxygen evolution reaction (OER) performance. Enhanced OER activity for mixed-metal spinel-type sulfide (CuCo2S4) nanorods is generally done by blending the material that has high conductive supports together with those having a high surface volume ratio, for example, graphitic carbon nitrides (g-C3N4). Here, we report a noble-metal-free CuCo2S4 nanorod-based electrocatalyst appropriate for basic OER and neutral media, through a simple one-step thermal decomposition approach from its molecular precursors pyrrolidine dithiocarbamate-copper(II), Cu[PDTC]2, and pyrrolidine dithiocarbamate-cobalt(II), Co[PDTC]2 complexes. Transmission electron microscopy (TEM) images as well as X-ray diffraction (XRD) patterns suggest that as-synthesized CuCo2S4 nanorods are highly crystalline in nature and are connected on the g-C3N4 support. Attenuated total reflectance-Fourier-transform infrared (ATR-FTIR), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy studies affirm the successful formation of bonds that bridge (Co-N/S-C) at the interface of CuCo2S4 nanorods and g-C3N4. The kinetics of the reaction are expedited, as these bridging bonds function as an electron transport chain, empowering OER electrocatalytically under a low overpotential (242 mV) of a current density at 10 mA cm-2 under basic conditions, resulting in very high durability. Moreover, CuCo2S4/g-C3N4 composite nanorods exhibit a high catalytic activity of OER under a neutral medium at an overpotential of 406 mV and a current density of 10 mA cm-2. � 2021 American Chemical Society.