关键词:
电催化硝酸盐还原
电催化亚硝酸盐还原
合成氨
合金化
异质结
摘要:
氨作为一种多用途化合物,在人类社会生活中发挥着重要作用。目前,氨的大规模生产依赖于能源密集型的Haber-Bosch工艺,这一工艺需要在高温高压的条件下进行,导致了巨大的能源消耗和环境负担。电合成技术是能在常温常压下生产氨的绿色合成工艺,电催化硝酸盐/亚硝酸盐还原合成氨(eNOxRR, x = 3和2)不仅可以解决环境污染问题,还能变废为宝,将污染物转化为高附加值产品。近几年来,eNOxRR催化剂的研究取得了一系列进展,其中铁基催化剂具有最大的电催化硝酸盐/亚硝酸盐还原合成氨潜力。然而,eNOxRR是一个复杂的多电子和多质子转移反应,反应过程中可能生成大量的副产物。同时,竞争性析氢反应会导致电子消耗和相对较低的选择性。因此eNOxRR系统的氨产率和法拉第效率仍有较大的提升空间。As a versatile compound, ammonia plays an important role in human social life. At present, the large-scale production of ammonia relies on the energy-intensive Haber–Bosch process, which requires reaction conditions of high temperature and pressure, resulting in huge energy consumption and environmental burden. Electrosynthesis technology is a green synthesis process that can produce ammonia at room temperature and pressure. Electrocatalytic nitrate/nitrite reduction to ammonia (eNOxRR, x = 3 and 2) can not only solve environmental pollution problems, but also turn waste into treasure and convert pollutants into high-value-added products. In recent years, research on eNOxRR catalysts has made a series of progress, among which iron-based catalysts have the greatest potential for electrocatalytic nitrate/nitrite reduction to ammonia. However, eNOxRR is a complex multi-electron and multi-proton transfer reaction, and a large number of byproducts can be generated. Meanwhile, competitive hydrogen evolution reaction results in electron consumption and relatively low selectivity. Therefore, there is still significant room for improvement of the ammonia yield rate and Faradaic efficiency of eNOxRR systems.