Peacock Scholarship

Surface Properties of Nanohybrid Water-Oxidation Electrocatalysts for Applications in Green Hydrogen Production

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The increase in the carbon dioxide emissions (CO2) from the burning of fossil fuels has led to environmental concerns due to global warming and escalating global climate change. One of the key solutions towards a sustainable future is to switch to renewable energy sources such as wind and solar energy which are clean and abundant. However since these resources are intermittent, it is critical to convert and store solar energy as chemical fuels. Artificial photosynthesis involves converting solar energy into chemical fuel, similar to how plants use photosynthesis to store solar energy into energy-rich sugar molecules. One major challenge in developing this technology is to discover robust water-oxidation catalysts (WOCs) that can efficiently oxidize water and produce oxygen, electrons and protons under a highly oxidizing environment. Water-splitting into hydrogen and oxygen can occur in a photoelectrochemical cell by interfacing the WOC to the anode and proton reduction catalyst (PRC) to the cathode. The traditional approach for wiring a WOC to an anode typically relies on the modification of the catalyst to incorporate anchoring groups, such as carboxylic acids or phosphonates. However, this can be synthetically challenging and these systems typically suffer from catalyst instability at pH ≥ 7. In this thesis work, we demonstrate a facile, versatile and simple method for the immobilization of an unmodified cationic ruthenium-based molecular complex RuCat1 (RuCat1 = [Ru(tpy)(bpy)(H2O)]2+, tpy =2,2’ : 6’2’’–terpyridine and bpy = 2,2’–bipyridine) to a grafted polymeric electrode surface. The surface polymer coating consisted of a UV crosslinked poly(acrylic acid) (PAA) network grafted into a conductive FTO (fluorine-doped tin-oxide) electrode. The immobilized Ru(II)-OEC|PAA|FTO films were characterized using various techniques, including attenuated total reflectance infrared spectroscopy (ATR-FTIR), UV-visible, cyclic voltammetry, and oxygen evolution studies which proves the successful attachment of the molecular WOC and point to a pH-dependent electrocatalytic activity.

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  • 06/13/2023
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