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水诱导固体电解质界面调控的连续流电化学合成氨
刘鹏博, 翟盛良, 黄继, 张衷硕, 曾杰, 李少锋
电化学(中英文)    2026, 32 (4): 2517001-.   DOI:10.61558/2993-074X.3605
摘要   (0 HTML12 PDF(pc) (2030KB)(437)  

连续流反应器可实现锂介导氮还原反应(Li-NRR)在常温常压下的连续运行,为替代哈伯-博施工艺提供了潜在方案。然而,该体系对电解液中痕量水分高度敏感,水含量的微小波动即会显著改变界面化学过程并影响反应性能。本研究系统考察了电解液初始水含量对连续流Li-NRR性能的影响机制。结果显示,过高的水含量会促进固体电解质界面层(SEI)增厚,阻碍氮气传质与锂离子传导,导致法拉第效率由61%骤降至3%。该机理认识揭示了痕量水在SEI演化中的关键调控作用,强调了精确控水对高效连续流Li-NRR的必要性。



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Fig. 5. Electrochemical testing of Li-NRR under varied water content in flow cells. (a, b) Chronopotentiometry curves at the water content of 5-7 mmol·L-1 (a) and 55-57 mmol·L-1 (b) respectively, recorded at a current density of -6 mA·cm-2 with an ethanol concentration of 43.0 mmol·L-1. (c) Chronopotentiometry curves of the first two cycles at varying water content in a flow cell. All reported potentials are presented without ohmic drop correction. (d) Nyquist plots of SEIs formed under varied water content, measured at room temperature. (e, f) First-cycle (e) and second-cycle (f) CV curves under different water content. (g) Long-term ammonia synthesis performed at an initial water content of 5-7 mmol·L-1. Insets show the Nyquist plot (left) and SEM image of the electrode after long-term operation (right). (h) Ammonia FE and electrolyte water content at cumulative charge passage during long-term experiments.
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