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机构地区:[1]南通大学化学化工学院,江苏 南通 [2]苏州大学能源学院,江苏 苏州
出 处:《物理化学进展》2024年第4期584-599,共16页Journal of Advances in Physical Chemistry
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 fo
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