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Boosting active hydrogen generation by anchored Ru sites in Co3O4 for nitrate-to-ammonia electrosynthesis
Chem Catalysis ( IF 11.5 ) Pub Date : 2024-10-17 , DOI: 10.1016/j.checat.2024.101152
Zhaole Lu, Rong Yang, Yingchao Yu, Yuting Wang, Bin Zhang, Lingjun Kong

The electrochemical reduction of nitrate to ammonia can serve as an effective complement to the traditional Haber-Bosch process. Currently, rapid and continuous ammonia production is challenging because of the multistep hydrogenation process and the constant alkalinization of the electrolyte. Herein, Ru atoms are incorporated into the octahedral sites of Co3O4 to achieve an ammonia yield rate of 24.6 mg h−1 cm−2. Electrochemical in situ spectroscopic analyses and theoretical calculations reveal that Ru sites improve water molecule coverage and facilitate the production of active hydrogen atoms, leading to stable and orderly ammonia production. Furthermore, a peak power density of 32.28 mW cm−2, a high ammonia Faradaic efficiency of 98.2%, and excellent durability (91 h) are achieved in a Ru-Co3O4-based Zn-nitrate battery, indicating its practical applicability. This work may provide a method for efficient nitrate reduction to ammonia or other hydrogenation reactions via the synergistic modulation of active sites.

中文翻译:


通过在 Co3O4 中锚定 Ru 位点促进活性氢的产生,用于硝酸盐-氨电合成



硝酸盐电化学还原为氨可以作为传统 Haber-Bosch 工艺的有效补充。目前,由于多步加氢过程和电解质的持续碱化,快速和连续的氨生产具有挑战性。在此,Ru 原子被掺入 Co3O4 的八面体位点,以实现 24.6 mg h-1 cm-2 的氨产率。电化学位光谱分析和理论计算表明,Ru 位点提高了水分子的覆盖率,促进了活性氢原子的产生,从而实现了稳定有序的氨生产。此外,基于 Ru-Co3O4 的硝酸锌电池实现了 32.28 mW cm-2 的峰值功率密度、98.2% 的高氨法拉第效率和出色的耐用性 (91 h),表明其实际适用性。这项工作可能提供一种通过活性位点的协同调节将硝酸盐高效还原为氨或其他氢化反应的方法。
更新日期:2024-10-17
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