电化学
氨
催化作用
无机化学
材料科学
化学
氮气
氢
铜
硝酸盐
电子转移
氨生产
电极
光化学
物理化学
有机化学
作者
Gao‐Feng Chen,Yifei Yuan,Haifeng Jiang,Shiyu Ren,Liang‐Xin Ding,Lu Ma,Tianpin Wu,Jun Lü,Haihui Wang
出处
期刊:Nature Energy
[Springer Nature]
日期:2020-07-27
卷期号:5 (8): 605-613
被引量:739
标识
DOI:10.1038/s41560-020-0654-1
摘要
Ammonia (NH3) is essential for modern agriculture and industry and is a potential energy carrier. NH3 is traditionally synthesized by the Haber–Bosch process at high temperature and pressure. The high-energy input of this process has motivated research into electrochemical NH3 synthesis via nitrogen (N2)–water reactions under ambient conditions. However, the future of this low-cost process is compromised by the low yield rate and poor selectivity, ascribed to the inert N≡N bond and ultralow solubility of N2. Obtaining NH3 directly from non-N2 sources could circumvent these challenges. Here we report the eight-electron direct electroreduction of nitrate to NH3 catalysed by copper-incorporated crystalline 3,4,9,10-perylenetetracarboxylic dianhydride. The catalyst exhibits an NH3 production rate of 436 ± 85 μg h−1 cm−2 and a maximum Faradaic efficiency of 85.9% at −0.4 V versus a reversible hydrogen electrode. This notable performance is achieved by the catalyst regulating the transfer of protons and/or electrons to the copper centres and suppressing hydrogen production. Electrochemically reducing nitrogen-containing molecules could provide less energy-intense routes to produce ammonia than the traditional Haber–Bosh process. Here the authors use a catalyst comprising Cu embedded in an organic molecular solid to synthesize ammonia from nitrate ions.
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