Abstract

This study investigated the effect of H2S concentration (5, 10 and 50 ppm) on the degradation and performance of Ni-YSZ anode supported solid oxide fuel cells. When supplied with hydrogen fuel containing H2S, the cell voltage dropped rapidly, and with increasing H2S concentration, voltage drop % increased (due to higher sulfur coverage on the Ni surface) and saturated more rapidly. A high concentration (50 ppm) of H2S led to an additional, slow rate voltage loss. In all cases, cell performance did not completely recover even after being supplied with H2S-free hydrogen fuel, because of the incomplete desorption of sulfur from the Ni surface. After the performance tests, nickel sulfides were detected on the Ni surface by Raman spectra, which were produced by the reaction of the remaining adsorbed sulfur with Ni during the cooling process. This indicates that the formation of nickel sulfides was not responsible for the secondary voltage drop. SEM/EDS analyses combined with FIB revealed that the reason for the additional 2nd drop was Ni oxidation; at a high sulfur coverage ratio (50 ppm), the outer layer of the Ni particle was oxidized by oxygen ions transported from the electrolyte. This indicates that H2S concentration as well as current density is a critical factor for Ni oxidation, and gives rise to the second voltage drop (irreversible cell degradation). The present work showed that the degradation behavior and phenomenon can differ significantly depending on the concentration of H2S, i.e., permanent changes may or may not occur on the anode (such as Ni oxidation) depending upon H2S concentration.

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