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Unique Hollow Ni-Fe@MoS2 Nanocubes with Boosted Electrocatalytic Activity for N2 Reduction to NH3

Abstract

Nanostructure tailoring is being thought as an efficient strategy to design high-performance electrocatalysts for improving electrocatalytic properties by exposing more active sites and promoting rapid electron transfer. Unfortunately, well-constructed morphology of nanomaterials on the nitrogen reduction reaction (NRR) at ambient conditions is urgently insufficient, and the yields 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 this 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 0.1 M Na2SO4 electrolyte, this as-prepared Ni-Fe@MoS2 NCs exhibits significant NH3 yield of 128.17 μg h-1 mgcat.-1 and satisfied Faradaic efficiency of 11.34% at -0.3 V vs. reversible hydrogen electrode (RHE) operation at 40℃. The stability of the catalyst was performed by 20-hour continuous N2 reduction with a constant current density. The possible NRR catalytic paths, mechanism and electrons 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.

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Supplementary files

Article information


Submitted
05 Dec 2019
Accepted
24 Mar 2020
First published
24 Mar 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

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, Accepted Manuscript , DOI: 10.1039/C9TA13336D

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