Rigid anchoring of highly crystallized and uniformly dispersed Pd nanocrystals on carbon fibers for ambient electrocatalytic reduction of nitrogen to ammonia
- 13 April 2021
- journal article
- research article
- Published by Royal Society of Chemistry (RSC) in Dalton Transactions
- Vol. 50 (20) , 6975-6981
Abstract
Developing efficient and stable electrocatalysts for ammonia synthesis via the nitrogen reduction reaction (NRR) is essential for the Earth's nitrogen cycle. Herein, a palladium nanocrystals anchored carbon fibers (PdNCs@CNFs) composite was prepared via electrospinning and carbonization processes. X-ray diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) characterization studies show that the as-prepared Pd grains are homogeneously anchored on the outer/inner section of the carbon nanofibers. Benefiting from the sufficient exposure and stress effect of active sites, the resultant PdNCs@CNFs achieves a high Faraday efficiency of ∼14.8% with a current density of 0.028 mA cm−2 at −0.2 V vs. reversible hydrogen electrode (RHE) in 0.1 M Na2SO4 solution, surpassing those of many catalysts previously reported. Density functional theory (DFT) calculations reveal that the rationality of the distal associative mechanism on PdNCs@CNFs and Pd nanocrystals on the surface of PdNCs@CNFs is more favorable for nitrogen (N2) molecule adsorption and polarization.Keywords
Funding Information
- Natural Science Foundation of Shanxi Province (201801D121059)
- National Natural Science Foundation of China (21878201, 22008165 and 51702279)
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