Format:
1 Online-Ressource (23 p)
Content:
Electrochemical N 2 reduction to NH 3 offers a mild and feasible alternative to Haber-Bosch NH 3 synthesis. Designing a promising NRR catalyst under alkaline conditions is highly desirable due to the advantages of alkaline electrolyte in fast charge transfer and limiting the hydrogen evolution reaction. However, the ammonia yield rate of iron catalysts is lower, usually below 40 µg h −1 mg −1 cat. Herein, the Fe-B/NC catalyst is synthesized by the pre-polymerization and pyrolysis processes. This catalyst exhibited a NH 3 yield 88.7 µg h −1 mg −1 cat at −0.45 V vs. RHE an alkaline electrolyte, which is greater than those values reported in the literature. Combining experimental analysis with DFT calculations, we demonstrate that the introduction of B coordination breaks the symmetric electron distribution of FeN 4 strategy so as to regulate its N 2 adsorption,activation and thus the NRR performance. B dopant induces the formation of electron-rich Fe, which is in favor of generating suitable adsorption and facilitating activation of N 2 molecules
Language:
English
DOI:
10.2139/ssrn.4037947
