Abstract
The electrocatalytic reduction reaction of carbon dioxide can be significantly enhanced by the use of sharp tip electrode. However, the experimentally observed rate enhancement is many orders of magnitudes smaller than what one would expect from an energetic point of view. Here we demonstrate that the kinetic of this tip-enhanced reaction plays a decisive role by proposing a novel reaction-diffusion kinetic model. The experimentally observed sharp-tip enhanced reaction and the maximal producing rate of carbon monoxide under different electrode potentials are well reproduced. Moreover, the optimal performance shows a strong dependence on the interaction between CO2 and the local electric field, on the adsorption rate of CO2, but not on the reaction barrier. Two new strategies to further enhance the reaction rate have also been proposed. Our findings highlight the importance of the kinetic in modeling electrocatalytic reactions.
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