Electrocatalytic Synthesis of Ammonia at Room Temperature and Atmospheric Pressure from Water and Nitrogen on a Carbon‐Nanotube‐Based Electrocatalyst

作者：Shiming Chen, Siglinda Perathoner, Claudio Ampelli, Chalachew Mebrahtu, Dangsheng Su, Gabriele Centi · 发表于：Angewandte Chemie International Edition · 年份：2017 · DOI：10.1002/anie.201609533 · 被引用次数：617 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Hydrogen Storage and Materials、Advanced Photocatalysis Techniques

Abstract Ammonia is synthesized directly from water and N2 at room temperature and atmospheric pressure in a flow electrochemical cell operating in gas phase (half‐cell for the NH3 synthesis). Iron supported on carbon nanotubes (CNTs) was used as the electrocatalyst in this half‐cell. A rate of ammonia formation of 2.2×10−3 g m−2 h−1 was obtained at room temperature and atmospheric pressure in a flow of N2, with stable behavior for at least 60 h of reaction, under an applied potential of −2.0 V. This value is higher than the rate of ammonia formation obtained using noble metals (Ru/C) under comparable reaction conditions. Furthermore, hydrogen gas with a total Faraday efficiency as high as 95.1 % was obtained. Data also indicate that the active sites in NH3 electrocatalytic synthesis may be associated to specific carbon sites formed at the interface between iron particles and CNT and able to activate N2, making it more reactive towards hydrogenation.