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The intermediate valence state Mo5+ in Fe doping La2(MoO4)3 boosting electrochemical nitrogen reduction
Journal of Power Sources ( IF 9.2 ) Pub Date : 2024-04-30 , DOI: 10.1016/j.jpowsour.2024.234621
Liangqing Hu , Yanming Guo , Yinpeng Lu , Jin Chang , Xiaojiang Su , Xinyi Zhang , Tong Wei , Hexin Zhang , Jing Feng

NH is considered as an ideal fuel for fuel cells to achieve zero carbon emissions due to its high energy density (at liquefaction) and carbon-free properties. The zero-carbon clean electrocatalytic nitrogen reduction reaction (NRR) is one of the alternative routes for NH synthesis. The efficiency of NRR is restricted by the high stability of N N and the slow reaction rate. In this study, La(MoO) (LaMo), and x%Fe doping-LaMo (x = 3, 5, 7, and 10) are synthesized via a hydrothermal method. The strong electron-donating ability of Fe converts a part of Mo to Mo and Mo improving the electronic environment. The presence of Mo, an intermediate valence state, facilitates the oxidation and reduction reactions and establishes rapid electron transport channels. The electron transport of is easier than . Furthermore, the Mo activates N and enhances N adsorption, boosting the NRR performance. Importantly, the content of Mo exhibits a positive correlation with NH yield rate ( = 0.89), and Faradaic efficiency (FE, = 0.95). Consequently, the 5%Fe–LaMo exhibits the highest Mo percentage (75.9 %) and NRR performance (NH yield rate:30.4 μg h mg, FE: 3.6 %). Thus, this study proposes a method to enhance the NRR performance by element doping with strong electron-donating ability to regulate the Mo percentage.

中文翻译:

Fe掺杂La2(MoO4)3中的中间价态Mo5+促进电化学氮还原

由于其高能量密度(液化时)和无碳特性,NH被认为是燃料电池实现零碳排放的理想燃料。零碳清洁电催化氮还原反应(NRR)是NH合成的替代路线之一。 NRR的效率受到NN的高稳定性和缓慢的反应速率的限制。在本研究中,通过水热法合成了 La(MoO) (LaMo) 和 x%Fe 掺杂-LaMo (x = 3、5、7 和 10)。 Fe的强给电子能力将部分Mo转化为Mo,Mo改善了电子环境。 Mo(中间价态)的存在促进氧化和还原反应并建立快速电子传输通道。的电子传输比 更容易。此外,Mo 还可以激活 N 并增强 N 吸附,从而提高 NRR 性能。重要的是,Mo 含量与 NH 产率 (= 0.89) 和法拉第效率 (FE = 0.95) 呈正相关。因此,5%Fe-LaMo 表现出最高的 Mo 百分比 (75.9%) 和 NRR 性能(NH 产率:30.4 μg h mg,FE:3.6%)。因此,本研究提出了一种通过强给电子能力的元素掺杂来调节Mo含量来增强NRR性能的方法。
更新日期:2024-04-30
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