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Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions
Chem ( IF 23.5 ) Pub Date : 2020-02-13 , DOI: 10.1016/j.chempr.2020.01.013
Jie Li , Shang Chen , Fengjiao Quan , Guangming Zhan , Falong Jia , Zhihui Ai , Lizhi Zhang

Electrocatalytic N2 reduction reaction (NRR) offers a promising low-energy, sustainable ammonia-synthesizing alternative to Haber-Bosch reaction. One roadblock lying in access to high-performance ammonia electrosynthesis emanates from the unsatisfied ability of electrocatalysts to wreck N≡N bond. Here, we report that interfacial polarization is an efficient scenario to enhance N≡N fracture to boost electrocatalytic ammonia synthesis. As a proof-of-concept demonstration, protrusion-shaped Fe single-atom catalysts immobilized onto MoS2 nanosheets engender electric fields to polarize N2. The resultant interfacial polarization fields between Fe-MoS2 and N2 drive the injection of more electrons into N2 antibonding orbitals in a fast manner, leading to a superior ammonia-evolving rate (36.1 ± 3.6 mmol g−1 h−1 or 97.5 ± 6 μg h−1 cm−2) at low applied potential. Similar phenomena are applicable in Co-MoS2, Cu-MoS2, Rh-MoS2, or Ru-MoS2, suggesting the potential universality of our interfacial polarization concept in upgrading wide-scope catalysis.



中文翻译:

通过单原子突起触发的界面极化将二氮加速电还原为氨。

电催化N 2还原反应(NRR)提供了一种有希望的低能量,可持续的氨合成方法,可替代Haber-Bosch反应。获得高性能氨电合成的障碍之一是电催化剂破坏N≡N键的能力不令人满意。在这里,我们报告界面极化是增强N≡N断裂以促进电催化氨合成的有效方案。作为概念验证,固定在MoS 2纳米片上的突起形Fe单原子催化剂产生电场以极化N 2。Fe-MoS 2和N 2之间的界面极化场会驱动更多的电子注入N2个快速形成反键的轨道,在较低的施加电势下,氨析出速率较高(36.1±3.6 mmol g -1 h -1或97.5±6μgh -1 cm -2)。类似的现象适用于Co-MoS 2,Cu-MoS 2,Rh-MoS 2或Ru-MoS 2,这表明我们的界面极化概念在升级宽光谱催化方面具有潜在的普遍性。

更新日期:2020-02-13
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