氨
催化作用
反键分子轨道
氨生产
Atom(片上系统)
电子
原子轨道
纳米技术
材料科学
化学
化学物理
极化(电化学)
物理化学
物理
有机化学
量子力学
嵌入式系统
计算机科学
作者
Jie Li,Chen Shang,Fengjiao Quan,Guangming Zhan,Falong Jia,Zhihui Ai,Lizhi Zhang
出处
期刊:Chem
[Elsevier]
日期:2020-04-01
卷期号:6 (4): 885-901
被引量:247
标识
DOI:10.1016/j.chempr.2020.01.013
摘要
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.
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