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Surface modification is one of the effective strategies to control the morphology and electrocatalytic performance of noble metal/transition metal oxide matrix composite catalysts. In this work, we successfully introduced modification groups such as -NH, -COOH, and -SH on the surface of FeO using the hydrothermal method. It was found that when the modification group -COOH was introduced, the regular spherical morphology of FeO was still maintained in FeO-COOH, while FeO-COOH had a relatively smaller spherical particle size (≈155.9 nm). Due to its smaller particle size, FeO-COOH has a larger active area than FeO, exposing more active sites. The abundant active sites in FeO-COOH provide more nucleation and growth sites for Au particles, which is beneficial for the recombination between FeO-COOH and Au. In addition, the experimental results of exploring the effect of Au precursor dosage on the synthesis of the FeO-COOH@Au structure and performance show that the synthesized FeO-COOH@Au catalyst has higher electrocatalytic activity. Due to the larger electrochemically active surface area of the FeO-COOH@Au catalyst compared to those of FeO-COOH@Au and FeO-COOH@Au catalysts, the adsorption and activation of NO reactants were accelerated, thereby improving the electrocatalytic performance. Therefore, owing to the morphological and structural characteristics of FeO-COOH combined with the high activity of Au nanoparticles, the synthesized FeO-COOH@Au exhibits effective electrocatalytic activity in the electrocatalytic NORR synthesis of ammonia. At a voltage of -0.8 V ( RHE), the ammonia yield reached 2092.8 μg h mg and Faraday efficiency reached 81.2%. The findings of this work will enrich our understanding of the construction of efficient FeO@Au catalysts based on surface functionalization and help to design efficient electrocatalytic NORR catalysts for practical applications.
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http://dx.doi.org/10.1039/d4dt01956c | DOI Listing |