In:
Angewandte Chemie, Wiley, Vol. 132, No. 19 ( 2020-05-04), p. 7426-7431
Abstract:
The electrochemical nitrogen reduction reaction (NRR) is a promising energy‐efficient and low‐emission alternative to the traditional Haber–Bosch process. Usually, the competing hydrogen evolution reaction (HER) and the reaction barrier of ambient electrochemical NRR are significant challenges, making a simultaneous high NH 3 formation rate and high Faradic efficiency (FE) difficult. To give effective NRR electrocatalysis and suppressed HER, the surface atomic structure of W 18 O 49 , which has exposed active W sites and weak binding for H 2 , is doped with Fe. A high NH 3 formation rate of 24.7 μg h −1 mg cat −1 and a high FE of 20.0 % are achieved at an overpotential of only −0.15 V versus the reversible hydrogen electrode. Ab initio calculations reveal an intercalation‐type doping of Fe atoms in the tunnels of the W 18 O 49 crystal structure, which increases the oxygen vacancies and exposes more W active sites, optimizes the nitrogen adsorption energy, and facilitates the electrocatalytic NRR.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v132.19
DOI:
10.1002/ange.202002029
Language:
English
Publisher:
Wiley
Publication Date:
2020
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