Progress in the Electrochemical Synthesis of Ammonia
Progress in the Electrochemical Synthesis of Ammonia
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DOI：
10.1016/j.cattod.2016.06.014
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发表时间：
2017-05-15
期刊：
影响因子：
5.3
通讯作者：
Stoukides, M.
中科院分区：
文献类型：
--
作者：
Kyriakou, V.;Garagounis, I.;Stoukides, M.
氨是世界上最重要和最广泛生产的化学品之一，对人类人口的增长起着关键作用。目前，合成氨的主要路线是百年前发展起来的哈伯-博世工艺。在这一过程中，铁基催化剂通常在400至500摄氏度的温度和130至170巴的压力下使用。与工业过程相反，在自然界中，植物和细菌在温和的条件下生产氨已经有数百万年的历史了。大气中的氮被金属酶固氮酶的FeMo辅因子上的溶剂化质子还原。自然的固氮方法激发了几个研究小组探索常压下电化学氨的合成。自1998年首次展示以来，电化学合成已经在广泛的温度范围内(25800摄氏度)进行了各种实验配置的研究。本文综述了该方法在固体和液体电解槽中的研究进展。实验研究分为高温(T>；500℃)、中温(500℃；T>；100℃)和低温(T<；100℃)。实验观测结果与基于密度泛函理论计算的理论预测进行了对比讨论。分析了电化学法的技术经济利弊，以及实现实际应用所需满足的要求。(C)2016爱思唯尔B.V.保留所有权利。
Ammonia is one of the most important and widely produced chemicals worldwide with a key role in the growth of human population. Nowadays, the main route for ammonia synthesis is the Haber-Bosch process, developed a century ago. In this process, Fe-based catalysts are usually employed at temperatures between 400 and 500 degrees C and pressures between 130 and 170 bar. As opposed to the industrial process, in nature, plants and bacteria have been producing ammonia for millions of years at mild conditions. Atmospheric nitrogen is reduced by solvated protons on the FeMo cofactor of the metalloenzyme nitrogenase. The natural method of nitrogen fixation has motivated several research groups to explore the electrochemical synthesis of ammonia at ambient pressure. Since it was first demonstrated in 1998, the electrochemical synthesis has been studied in a variety of experimental configurations over a wide temperature range (25800 degrees C). In the present review, the progress of this method in both solid and liquid electrolyte cells is reported. The experimental studies are divided into high (T > 500 degrees C), intermediate (500 degrees C > T > 100 degrees C) and low (T < 100 degrees C) temperatures. The experimental observations are comparatively discussed with theoretical predictions based on DFT calculations. The techno-economic advantages and disadvantages of the electrochemical approach, as well as the requirements to be met in order to enable practical applications are also analyzed. (C) 2016 Elsevier B.V. All rights reserved.