On the promoting effect of H2S on the catalytic H2 production over Gd-doped ceria from CH4/H2O mixtures for solid oxide fuel cell applications

• Published in: Journal of catalysis Vol. 316; pp. 149 - 163
• Main Authors: Postole, G., Bosselet, F., Bergeret, G., Prakash, S., Gélin, P.
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier Inc 01.07.2014; Elsevier; Elsevier BV
• Subjects: Applied sciences; Catalysis; CH4/H2O reaction; Chemical engineering; Chemistry; Direct energy conversion and energy accumulation; Electrical engineering. Electrical power engineering; Electrical power engineering; Electrochemical conversion: primary and secondary batteries, fuel cells; Energy; Energy. Thermal use of fuels; Equipments for energy generation and conversion: thermal, electrical, mechanical energy, etc; Exact sciences and technology; Fuel cells; Gadolinium-doped ceria; General and physical chemistry; H2S; Heterogeneous catalysis; SOFC; Solid oxide fuel cells; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry; H2S; Heterogeneous catalysis; CH4/H2O reaction; Gadolinium-doped ceria; SOFC; Methane; Binary compound; Catalytic reaction; CH; H; Gadolinium; Hydrogen sulfides; Cerium oxide; Solid oxide fuel cell; Lanthanide compound; S; O reaction
• ISSN: 0021-9517; 1090-2694
• DOI: 10.1016/j.jcat.2014.05.011

[Display omitted] •A commercial Gd-doped ceria powder (CGO) shows higher activity during CH4/H2O reaction in the presence of H2S.•The improved activity was associated with the formation and stabilization of oxygen vacancies by S-insertion in ceria lattice.•Increasing the H2S concentration may also induce Ce2O2S formation detrimental to the catalytic activity. In order to understand the exceptional tolerance of ceria to high sulfur levels in the fuel for further SOFC applications, the interaction of sulfur with a commercial Ce0.9Gd0.1O2−x (CGO, from Praxair) and its influence on H2 production from CH4/H2O mixture was studied. The activity tests were performed at 750°C, in the presence of H2S and under gradual internal reforming conditions (large excess of CH4 with respect to water vapor, 10:1). The presence of H2S in the reactant mixture promoted the catalytic activity of CGO. The nature of various species formed by sulfur–ceria interaction is discussed based on CH4-TPR, XRD, XPS, and in situ FTIR results. H2S reacts with ceria fraction in CGO and generates new catalytic sites with improved reactivity toward CH4. The formation and stabilization of oxygen vacancies by S-insertion in ceria lattice are evidenced and directly related to the improved activity. The detrimental effect of Ce2O2S phase, when formed, on the catalytic activity of doped ceria is confirmed.