Department of Chemistry, University of California, 1 Shields Ave, Davis, CA, 95616, USA.
Chemistry. 2019 Jan 7;25(2):454-458. doi: 10.1002/chem.201804454. Epub 2018 Oct 30.
Electrochemical generation of ammonia (NH ) from nitrogen (N ) using renewable electricity is a desirable alternative to current NH production methods, which consume roughly 1 % of the world's total energy use. The use of catalysts to manipulate the required electron and proton transfer reactions with low energy input is also a chemical challenge that requires development of fundamental reaction pathways. This work presents an approach to the electrochemical reduction of N into NH using a coordination complex of aluminum(III), which facilitates NH production at -1.16 V vs. SCE. Reactions performed under N liberate NH . Electron paramagnetic resonance spectroscopic characterization of a reduced intermediate and investigations of product inhibition, which limit the reaction to sub-stoichiometric, are also presented.
用电能将氮气（N ）电化学转化为氨（NH ）是一种替代当前氨生产方法的理想选择，因为当前的方法消耗了全球总能源使用量的约 1%。使用催化剂以低能量输入来操纵所需的电子和质子转移反应也是一个化学挑战，需要开发基本的反应途径。这项工作提出了一种使用三价铝（III）配合物电化学还原 N 生成 NH 的方法，该方法在相对于 SCE 为-1.16 V 的电势下促进 NH 的生成。在 N 存在下进行的反应会释放出 NH 。还介绍了还原中间产物的电子顺磁共振波谱表征以及对产物抑制的研究，产物抑制会将反应限制为亚化学计量。
