Journal
CHEMICAL ENGINEERING JOURNAL
Volume 417, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2020.127924
Keywords
Interstitial doping; Mo2C Faradaic efficiency; Nitrogen reduction; Electrocatalyst
Categories
Funding
- National Key Research Development Program of China [2019YFB2203503]
- National Natural Science Foundation of China [61875138, 61435010, 61961136001]
- Science and Technology Innovation Commission of Shenzhen [KQTD2015032416270385, JCYJ20170811093453105, JCYJ20180307164612205, GJHZ20180928160209731]
- Instrumental Analysis Center of Shenzhen University (Xili Campus)
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The study developed a novel electrocatalyst for improving the efficiency of ammonia synthesis through theoretical calculations and experimental methods, which showed high Faradaic efficiency and ammonia yield rate, along with excellent stability.
The electrochemical nitrogen reduction reaction (eNRR) provides a sustainable way to generate ammonia (NH3) but its Faradaic efficiency (FE) is relatively low and could be further improved, especially on the highly active molybdenum carbide (Mo2C) electrocatalyst. Our theoretical calculations suggest that unlike substitute doping model, interstitial Fe doping into Mo2C is highly eNRR-selective due to decreasing hydrogen evolution activity and unique surface-hydrogenation mechanism on negatively charged Mo sites around Fe atoms. Inspired by this prediction, we successfully developed a novel interstitial Fe doped Mo2C electrocatalyst by the pyrolysis of Fedoped Mo/Zn bimetallic imidazolate frameworks (Fe-Mo/Zn BIFs) as a precursor where Fe atoms substitute Zn sites to obtain the spatial confinement effect. When evaluated in eNRR catalysis, Fe/Mo2C catalyst therefore exhibits a much higher FE of 20.1% at 0.45 V vs. RHE (reversible hydrogen electrode), which is almost double that of pristine Mo2C and substitute type. Moreover, the Fe/Mo2C catalyst also exhibits high ammonia yield rate with excellent durability over the six continuous cycles.
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