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Hydrogen gas is a promising renewable energy storage medium when produced via water electrolysis, but this process is limited by the sluggish kinetics of the anodic oxygen evolution reaction (OER). Herein, we used a microkinetic model to investigate promoting the OER using programmable oxide catalysts (i.e., forced catalyst dynamics). We found that programmable catalysts could increase current density at a fixed overpotential (100-600× over static rates) or reduce the overpotential required to reach a fixed current density of 10 mA cm-2 (45-140% reduction vs static). In our kinetic parametrization, the key parameters controlling the quality of the catalytic ratchet were the O*-to-OOH* and O*-to-OH* activation barriers. Our findings indicate that programmable catalysts may be a viable strategy for accelerating the OER or enabling lower-overpotential operation, but a more accurate kinetic parametrization is required for precise predictions of performance, ratchet quality, and resulting energy efficiency.more » « less
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Temples, Spencer C.; Gathmann, Sallye R.; Ding, Junhuan; Thies, Mark C. (, Industrial & Engineering Chemistry Research)
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Onn, Tzia Ming; Gathmann, Sallye R.; Wang, Yuxin; Patel, Roshan; Guo, Silu; Chen, Han; Soeherman, Jimmy K.; Christopher, Phillip; Rojas, Geoffrey; Mkhoyan, K. Andre; et al (, JACS Au)
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