Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts.

Yin, Di; Li, Bowen; Gao, Boxiang; Chen, Mengxue; Chen, Dong; Meng, You; Zhang, Shuai; Zhang, Chenxu et al. · Adv Mater · 2025

basic_science · Level V

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Abstract

Electrochemically converting nitrate (NO<sub>3</sub> <sup>-</sup>) to value-added ammonia (NH<sub>3</sub>) 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 NH<sub>3</sub> electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5 ± 4.3% and a yield rate of 10.2 ± 0.5 mg h<sup>-1</sup> mg<sub>cat</sub> <sup>-1</sup>. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH<sub>3</sub> 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.