Ammonia (NH₃) is an energy carrier that can be synthesized from nitrogen and water using electricity generated from renewable sources. The present work investigated NH₃ synthesis using an electrochemical system with the structure of Ru/Cs⁺/MgO|Pd–Ag|CsH₂PO₄/SiP₂O₇|Pt and operating at 200 to 250 °C. In this system, the NH₃ being generated is isolated from the CsH₂PO₄/SiP₂O₇ electrolyte by the hydrogen-permeable Pd–Ag membrane, resulting in the production of dry NH₃. A maximum NH₃ synthesis rate of 0.90 nmol s⁻¹ cm⁻² was obtained from the cathode at the Ru/Cs⁺/MgO|Pd–Ag side at a current density of 10 mA cm⁻², temperature of 250 °C and N₂ flow rate of 3 cm³ min⁻¹ as converted to standard temperature and pressure. Deviations in the NH₃ production rate from the theoretical amounts predicted by Arrhenius plots were observed at temperatures approaching 250 °C, possibly because the reaction approached equilibrium. A current efficiency for NH₃ production of 2.6% was obtained, with the remainder of the current consumed during H₂ generation. The apparent activation energies for the NH₃ synthesis were 69 and 93 kJ mol⁻¹ at 3.2 and 10 mA cm⁻², respectively. These values are significantly lower than that reported for conventional NH₃ synthesis from nitrogen and hydrogen (139 kJ mol⁻¹) over the same catalyst in this cell. The optimum N₂ flow rates were approximately 0.5 and 5 cm³ min⁻¹ at 3.2 and 10 mA cm⁻², respectively, representing nitrogen amounts approximately 42 times the stoichiometric quantities. The provision of an excess of N₂ is believed to reduce the suppression of N₂ activation by so-called hydrogen poisoning of the catalyst.

中文翻译：

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使用Ru催化剂，氢可渗透的Pd膜和磷酸盐基电解质在200至250°C的温度下通过电解从N ₂和H ₂ O合成NH _3的电化学膜电池

氨（NH ₃）是一种能源载体，可以使用可再生资源产生的电能由氮和水合成。本工作研究了使用Ru / Cs ⁺ / MgO | Pd–Ag | CsH ₂ PO ₄ / SiP ₂ O ₇ | Pt结构的电化学系统在200至250°C的温度下合成NH _3的过程。在该系统中，通过氢可渗透的Pd-Ag膜从CsH ₂ PO ₄ / SiP ₂ O ₇电解质中分离出正在生成的NH ₃，从而产生干燥的NH ₃。最高NH ₃在10 mA cm ^-2的电流密度，250°C的温度和N ₂流速下，从Ru / Cs ⁺ / MgO | Pd-Ag侧的阴极获得0.90 nmol s ^-1 cm ^-2的合成速率3 cm ³ min ^-1转换为标准温度和压力。在接近250°C的温度下，观察到NH ₃生成速率与Arrhenius图所预测的理论量存在偏差，这可能是因为反应已趋于平衡。NH ₃生产的电流效率为2.6％，其余电流在H ₂期间消耗一代。NH ₃合成的表观活化能在3.2和10mA cm ^-2分别为69和93kJ mol ^-1。这些值明显低于在该电池中的相同催化剂上由氮气和氢气（139 kJ mol ^-1）合成常规NH _3的报告值。最佳N ₂流速分别为3.2和10 mA cm ^-2时分别约为0.5和5 cm ³ min ^-1，代表氮含量约为化学计量的42倍。认为提供过量的N ₂减少了对N ₂的抑制。 通过所谓的催化剂氢中毒而活化。