Issue 15, 2020

Unique hollow Ni–Fe@MoS2 nanocubes with boosted electrocatalytic activity for N2 reduction to NH3

Abstract

Nanostructure tailoring is considered as an efficient strategy to design high-performance electrocatalysts for improving electrocatalytic properties by exposing more active sites and promoting rapid electron transfer. Unfortunately, nanomaterials with a well-constructed morphology for the nitrogen reduction reaction (NRR) under ambient conditions are insufficient, and the yield rate and faradaic efficiency are still not high. Herein, NiFe–MoS2 nanocubes (NiFe@MoS2 NCs) are successfully synthesized derived from the corresponding Prussian blue analog self-templating strategy. Owing to its four-pointed star face-dependent hollow structure and trimetallic synergistic interactions, it largely exposes abundant active sites, making it present superb electrocatalytic performance for N2 conversion to NH3. In a 0.1 M Na2SO4 electrolyte, these as-prepared Ni–Fe@MoS2 NCs exhibit a significant NH3 yield of 128.17 μg h−1 mgcat.−1 and a satisfactory faradaic efficiency of 11.34% at −0.3 V vs. reversible hydrogen electrode (RHE) operation at 40 °C. The stability of the catalyst was determined by performing 15 hour continuous N2 reduction with a constant current density. The possible NRR catalytic paths, mechanism and electron transfer paths are elucidated in detail by in situ electrochemical-Fourier transform infrared spectroscopy combined with density functional theory calculations. This work offers new inspirations to the development of various cost-effective electrocatalysts for N2 fixation.

Graphical abstract: Unique hollow Ni–Fe@MoS2 nanocubes with boosted electrocatalytic activity for N2 reduction to NH3

Supplementary files

Article information

Article type
Paper
Submitted
05 Dec 2019
Accepted
24 Mar 2020
First published
24 Mar 2020

J. Mater. Chem. A, 2020,8, 7339-7349

Unique hollow Ni–Fe@MoS2 nanocubes with boosted electrocatalytic activity for N2 reduction to NH3

L. Zeng, X. Li, S. Chen, J. Wen, W. Huang and A. Chen, J. Mater. Chem. A, 2020, 8, 7339 DOI: 10.1039/C9TA13336D

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