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Non-aqueous gas diffusion electrodes for rapid ammonia synthesis from nitrogen and water-splitting-derived hydrogen
Nature Catalysis ( IF 42.8 ) Pub Date : 2020-05-04 , DOI: 10.1038/s41929-020-0455-8
Nikifar Lazouski , Minju Chung , Kindle Williams , Michal L. Gala , Karthish Manthiram

Electrochemical transformations in non-aqueous solvents are important for synthetic and energy storage applications. Use of non-polar gaseous reactants such as nitrogen and hydrogen in non-aqueous solvents is limited by their low solubility and slow transport. Conventional gas diffusion electrodes improve the transport of gaseous species in aqueous electrolytes by facilitating efficient gas–liquid contacting in the vicinity of the electrode. Their use with non-aqueous solvents is hampered by the absence of hydrophobic repulsion between the liquid phase and carbon fibre support. Herein we report a method to overcome transport limitations in tetrahydrofuran using a stainless steel cloth-based support for ammonia synthesis paired with hydrogen oxidation. An ammonia partial current density of 8.8 ± 1.4 mA cm−2 and a Faradaic efficiency of 35 ± 6% are obtained using a lithium-mediated approach. Hydrogen oxidation current densities of up to 25 mA cm−2 are obtained in two non-aqueous solvents with near-unity Faradaic efficiency. The approach is then applied to produce ammonia from nitrogen and water-splitting-derived hydrogen.



中文翻译:

非水气体扩散电极,用于从氮气和水分解氢中快速合成氨

非水溶剂中的电化学转化对于合成和储能应用非常重要。非极性气态反应物(例如氮气和氢气)在非水溶剂中的使用受到其低溶解度和缓慢运输的限制。常规的气体扩散电极通过促进电极附近的有效气液接触来改善水性电解质中气态物质的传输。由于在液相和碳纤维载体之间不存在疏水斥力,因此阻碍了它们与非水溶剂的使用。在本文中,我们报告了一种方法,该方法使用不锈钢布基支持物用于氨合成以及氢氧化来克服四氢呋喃中的运输限制。氨分电流密度为8.8±1.4 mA cm -2使用锂介导的方法可获得35±6%的法拉第效率。在两种非水溶剂中以接近统一的法拉第效率获得了高达25 mA cm -2的氢氧化电流密度。然后将该方法应用于由氮和水分解氢产生氨。

更新日期:2020-05-04
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