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Ruthenium-induced hydrolysis effect on Fe2O3 nanoarrays for high-performance electrochemical nitrate reduction to ammonia
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2024-03-19 , DOI: 10.1016/j.apcatb.2024.123967
Shumin Luo , Heng Guo , Tingsong Li , Haoran Wu , Fengying Zhang , Chun Tang , Guoxing Chen , Guidong Yang , Ying Zhou

Electrochemical nitrate reduction (NORR) to ammonia (NH) has become an attractive pathway for sewage remediation and ammonia synthesis. However, the NO electroreduction reaction remains hindered by the sluggish multi-proton involved steps without sufficient proton supply. Herein, we designed Ru nanoparticles (NPs) loaded onto ferric oxide nanoarrays (Ru-FeO) catalysts with hydrolysis effect for high-efficient NH production. Ru-FeO exhibits an impressive ammonia yield and faraday efficiency (209–329 μmol cm h and 45.2–72.8%, respectively). Ru-induced hydrolysis promotes the hydrogenation of the reaction intermediates in the process () by accelerating the generation of localized protons at the reactive sites. More importantly, this effect can further accelerate the H*-mediated indirect reduction pathway and the electron-mediated direct reduction pathway. These findings underscore the importance of relating NORR performance with nanometallic particles-supported electrodes to advance catalyst design and operation.

中文翻译:

钌诱导的 Fe2O3 纳米阵列水解效应用于高性能电化学硝酸盐还原成氨

电化学硝酸盐还原(NORR)生成氨(NH)已成为污水修复和氨合成的一种有吸引力的途径。然而,在没有足够质子供应的情况下,NO 电还原反应仍然受到缓慢的多质子参与步骤的阻碍。在此,我们设计了负载在氧化铁纳米阵列(Ru-FeO)催化剂上的Ru纳米颗粒(NP),该催化剂具有水解作用,可高效生产NH。 Ru-FeO 表现出令人印象深刻的氨产率和法拉第效率(分别为 209–329 μmol cm h 和 45.2–72.8%)。 Ru诱导的水解通过加速反应位点局部质子的产生来促进过程中反应中间体的氢化。更重要的是,这种效应可以进一步加速H*介导的间接还原途径和电子介导的直接还原途径。这些发现强调了将 NORR 性能与纳米金属颗粒负载电极联系起来以推进催化剂设计和操作的重要性。
更新日期:2024-03-19
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