In:
Angewandte Chemie International Edition, Wiley, Vol. 60, No. 37 ( 2021-09-06), p. 20331-20341
Kurzfassung:
The multimetallic sulfur‐framework catalytic site of biological nitrogenases allows the efficient conversion of dinitrogen (N 2 ) to ammonia (NH 3 ) under ambient conditions. Inspired by biological nitrogenases, a bimetallic sulfide material (FeWS x @FeWO 4 ) was synthesized as a highly efficient N 2 reduction (NRR) catalyst by sulfur substitution of the surface of FeWO 4 nanoparticles. Thus prepared FeWS x @FeWO 4 catalysts exhibit a relatively high NH 3 production rate of 30.2 ug h −1 mg −1 cat and a Faraday efficiency of 16.4 % at −0.45 V versus a reversible hydrogen electrode in a flow cell; these results have been confirmed via purified 15 N 2 ‐isotopic labeling experiments. In situ Raman spectra and hydrazine reduction kinetics analysis revealed that the reduction of undissociated hydrazine intermediates (M‐NH 2 ‐NH 2 ) on the surface of the bimetallic sulfide catalyst is the rate‐determing step for the NRR process. Therefore, this work can provide guidance for elucidating the structure–activity relationship of NRR catalysts.
Materialart:
Online-Ressource
ISSN:
1433-7851
,
1521-3773
DOI:
10.1002/anie.202104918
Sprache:
Englisch
Verlag:
Wiley
Publikationsdatum:
2021
ZDB Id:
2011836-3
ZDB Id:
123227-7
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