Wang Yingchao, Ma Zizai, Liu Kai, Yang Xiaowei, Wang Jianxing, Wang Xiaoguang
Laboratory of Advanced Materials and Energy Electrochemistry, Institute of New Carbon Materials, College of Materials Science & Engineering, Taiyuan University of Technology, Taiyuan, 030024, China.
Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan, 030024, China.
Dalton Trans. 2021 May 25;50(20):6975-6981. doi: 10.1039/d1dt00682g.
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.
