Promoting electrocatalytic nitrogen reduction to ammonia via Fe-boosted nitrogen activation on MnO2 surfaces

The electrocatalytic nitrogen (N2) reduction reaction is recognized as a green and sustainable approach for ammonia (NH3) synthesis alternative to the traditional industrial method – the Haber–Bosch process, while an efficient electrocatalysis of such a process is a prerequisite for N2 reduction. De...

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Published inJournal of materials chemistry. A, Materials for energy and sustainability Vol. 8; no. 27; pp. 13679 - 13684
Main Authors Huang, Ting, Liu, Zaichun, Zhang, Yu, Wang, Faxing, Wen, Juan, Wang, Chengyin, Hossain, Masud, Xie, Qingji, Yao, Shouzhuo, Wu, Yuping
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 01.01.2020
Subjects
Ammonia
Catalysts
Chemical reduction
Chemical synthesis
Density functional theory
Durability
Electrocatalysts
Electrolysis
Haber Bosch process
Hydrothermal reactions
Manganese
Manganese dioxide
Manganese oxides
Morphology
Nitrogen
Sodium sulfate
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Summary:The electrocatalytic nitrogen (N2) reduction reaction is recognized as a green and sustainable approach for ammonia (NH3) synthesis alternative to the traditional industrial method – the Haber–Bosch process, while an efficient electrocatalysis of such a process is a prerequisite for N2 reduction. Developing a cost-effective electrocatalyst for the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions with an excellent catalytic performance remains a great challenge. Here, we report a facile hydrothermal reaction to synthesize Fe-doped manganese oxide (MnO2) with a nanoneedle morphology as a cost-effective electrocatalyst for the NRR. It is verified that Fe plays a critical role in the NRR. This catalyst shows an excellent catalytic performance with a high faradaic efficiency of 16.8% and a high NH3 formation rate of 39.2 μg h−1 mgcat.−1 at −0.29 V vs. the reversible hydrogen electrode in 0.1 M Na2SO4, which are much higher than those of all reported Mn-based NRR catalysts and many other previously reported catalysts. This catalyst also shows excellent durability during electrolysis and recycling tests. In addition, the electrocatalyst mechanism is also assessed in combination with density functional theory.
ISSN:2050-7488
2050-7496
DOI:10.1039/c9ta13026h