期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 43, 页码 15541-15547出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201910658
关键词
ammonia synthesis; carbide; electrocatalysis; nitrogen fixation; nitrogen reduction reaction
资金
- National Natural Science Foundation of China [21776099, 41701359]
- Guangdong Special Support Program [2017TQ04N086]
- National Key R&D Program of China [2016YFA0202601]
We demonstrate a simple and effective chemical equilibrium regulation strategy to improve the efficiency of electrochemical ammonia synthesis by constructing electrochemical reaction system that works at significantly lower pressure than the Haber-Bosch process. Transferring the nitrogen reduction reaction from ambient conditions to a lightly pressurized environment not only accelerates the activation of the N equivalent to N triple bond but also inhibits the competing reaction of hydrogen evolution while promoting the dissolution and diffusion of nitrogen. The verification experiment of using well-designed Fe3Mo3C/C composite nanosheets as the nitrogen reduction catalyst shows that the lower pressure reaction system can improve the Faradaic current efficiency by one order of magnitude. Moreover, the comparatively low-pressure reaction system can greatly reduce the cell voltage of the ammonia synthesis reaction (up to 33 %) even at the relatively low pressure of 0.7 MPa, which is of significance for decreasing the energy consumption of electrochemical ammonia synthesis under mild conditions.
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