S掺杂促进Fe/N/C催化剂氧还原活性的实验与理论研究

doi:10.3866/PKU.WHXB201705088

Abstract

Abstract:

S doping in Fe/N/C non-precious metal catalysts is an effective approach to further improve their catalytic activity for the oxygen reduction reaction (ORR). However, the enhancement mechanism is not yet clear. Here, we synthesized an Fe/N/C catalyst using melamine-formaldehyde resin as the N and C precursors, CaCl₂ as the template, and FeCl₃ as the Fe precursor. The effects of S doping on the morphology, textural property, composition, and ORR catalytic activity were investigated by adding various amounts of KSCN as a precursor. Transmission electron microscopy (TEM) and N₂ adsorption-desorption isotherm results revealed that S prevented the growth of Fe-containing nanoparticles, and facilitated the formation of a porous structure, which increased both the catalyst surface area and mass transfer rate. X-ray photoelectron spectroscopy (XPS) results indicated that a suitable amount of S precursor led to a high doping level of S and provided the highest ORR activity. However, too much S in the precursor decreased the doping levels of both Fe and S, due to the formation of FeS, which could be completely removed by acid leaching. Density functional theory (DFT) calculations showed that the addition of S in an Fe-N₄ macrocycle could enhance the interaction strength of the Fe―O bond between the O₂ molecule or the intermediate OOHspecies and Fe in the Fe-N₄ structure, resulting in a significant decrease in the O―O bond energy, and may help in bond breaking in subsequent reactions, facilitating the ORR process.

Key words: Oxygen reduction reaction, Non-precious metal catalyst, Fe/N/C materials, S-doping, Density functional theory

Chi CHEN,Xue ZHANG,Zhi-You ZHOU,Xin-Sheng ZHANG,Shi-Gang SUN. Experimental Boosting of the Oxygen Reduction Activity of an Fe/N/C Catalyst by Sulfur Doping and Density Functional Theory Calculations[J].Acta Phys. -Chim. Sin., 2017, 33(9): 1875-1883.

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Experimental Boosting of the Oxygen Reduction Activity of an Fe/N/C Catalyst by Sulfur Doping and Density Functional Theory Calculations

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