Abstract
Electrochemically converting nitrate (NO3 -) to value-added ammonia (NH3) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH3 electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5±4.3% and a yield rate of 10.2±0.5mg h-1 mgcat -1. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH3 collection. This work elucidates the catalytic mechanisms of multi-functional HEA systems and offers new perspectives for optimizing multi-step reactions by circumventing adsorption-energy scaling limitations.
Published Version
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