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Regulating RuxMoy Nanoalloys Anchored on Porous Nitrogen-Doped Carbon via Domain-Confined Etching Strategy for Neutral Efficient Ammonia Electrosynthesis
Nano Letters ( IF 9.6 ) Pub Date : 2024-09-12 , DOI: 10.1021/acs.nanolett.4c03319
Xin Ge 1 , Ronglan Pan 1 , Haibo Xie 1 , Shiwei Hu 2 , Jili Yuan 1, 3
Affiliation  

Neutral electrochemical nitrate (NO3) reduction to ammonia involves sluggish and complex kinetics, so developing efficient electrocatalysts at low potential remains challenging. Here, we report a domain-confined etching strategy to construct RuxMoy nanoalloys on porous nitrogen-doped carbon by optimizing the Ru-to-Mo ratio, achieving efficient neutral NH3 electrosynthesis. Combining in situ spectroscopy and theoretical simulations demonstrated a rational synergic effect between Ru and Mo in nanoalloys that reinforces *H adsorption and lowers the energy barrier of NO3 hydrodeoxygenation for NH3 production. The resultant Ru5Mo5-NC surpasses 92.8% for NH3 selectivity at the potential range from −0.25 to −0.45 V vs RHE under neutral electrolyte, particularly achieving a high NH3 selectivity of 98.3% and a corresponding yield rate of 1.3 mg h–1 mgcat–1 at −0.4 V vs RHE. This work provides a synergic strategy that sheds light on a new avenue for developing efficient multicomponent heterogeneous catalysts.

中文翻译:


通过域限制刻蚀策略调控锚定在多孔氮掺杂碳上的 RuxMoy 纳米合金,用于中性高效氨电合成



中性电化学硝酸盐 (NO3) 还原为氨涉及缓慢而复杂的动力学,因此开发低电位的高效电催化剂仍然具有挑战性。在这里,我们报道了一种域限蚀刻策略,通过优化 Ru-to-Mo 比,在多孔氮掺杂碳上构建 RuxMoy 纳米合金,实现高效的中性 NH3 电合成。结合原位光谱和理论模拟证明了纳米合金中 Ru 和 Mo 之间的合理协同效应,增强了 *H 吸附并降低了 NO3 的能垒-加氢脱氧以生产 NH3。在中性电解质下,在 -0.25 至 -0.45 V 与 RHE 的电位范围内,所得的 Ru5Mo5-NC 对 NH3 选择性的选择性超过 92.8%,特别是实现了 98.3% 的高 NH3 选择性和相应的产率 1.3 mg h–1 mgcat–1在 -0.4 V vs RHE 下。这项工作提供了一种协同策略,为开发高效的多组分非均相催化剂开辟了一条新途径。
更新日期:2024-09-12
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