Publications by authors named "Aravind Vadakkayil"

The oxygen evolution reaction (OER) remains an important bottleneck for widespread implementation of a hydrogen economy. While improvements in the OER can be realized by spin polarizing the reaction intermediates, these methods often rely on applying external magnetic fields to ferromagnetic catalysts or by adsorbing chiral molecules onto the catalyst. Here, we show that the addition of chiral additives to the conductive binder supporting the catalysts enhances the selectivity for O formation and results in exceedingly high mass activities.

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This work presents a spectroscopic and photocatalytic comparison of water splitting using yttrium iron garnet (YFeO, YIG) and hematite (α-FeO) photoanodes. Despite similar electronic structures, YIG significantly outperforms widely studied hematite, displaying more than an order of magnitude increase in photocurrent density. Probing the charge and spin dynamics by ultrafast, surface-sensitive XUV spectroscopy reveals that the enhanced performance arises from (1) reduced polaron formation in YIG compared to hematite and (2) an intrinsic spin polarization of catalytic photocurrents in YIG.

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Continual progress in technologies that rely on water splitting are often hampered by the slow kinetics associated with the oxygen evolution reaction (OER). Here, we show that the efficiency of top-performing catalysts can be improved, beyond typical thermodynamic considerations, through control over reaction intermediate spin alignment during electrolysis. Spin alignment is achieved using the chiral induced spin selectivity (CISS) effect and the improvement in OER manifests as an increase in Faradaic efficiency, decrease in reaction overpotential, and change in the rate determining step for chiral nanocatalysts over compositionally analogous achiral nanocatalysts.

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