In situ QXAS study of sulfidation/oxidative regeneration reactions of zinc molybdate (ZnMoO4) and ZnO–MoO3 materials

• Published in: Physical chemistry chemical physics : PCCP 2019, Vol.21 (16), p.8569-8579
• Main Authors: Girard, Vincent, Chiche, David, Baudot, Arnaud, Bazer-Bachi, Delphine, Lemaitre, Laurent, Moizan-Baslé, Virginie, Rochet, Amélie, Briois, Valérie, Geantet, Christophe
• Format: Article
• Language: English
• Subjects: Data analysis; Evolution; Gas-solid reactions; Hydrogen sulfide; Molybdenum oxides; Molybdenum trioxide; Multivariate analysis; Natural gas; Reaction kinetics; Regeneration; Sulfidation; Sulfur removal; Transition metal oxides; Transition metals; Zinc oxide
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/c9cp01008d

Recent technologies such as those using coal, natural gas or biomass as fuel are often facing the challenge of removing H2S impurities. Among the various existing routes for sulfur removal, the conversion of transition metal oxides into sulfides is often considered for deep gas purification. The ideal regenerative system, preventing waste generation, should combine a high affinity material towards H2S and an easy way for its regeneration into the initial oxide form. The present paper describes the reactivity of the ZnMoO4 mixed oxide material and ZnO–MoO3 oxides mixture as potential candidates for the regenerative H2S sorption process. The use of the QXAS technique allowed us to get time resolved information about both sulfidation and oxidative regeneration processes at Mo and Zn K-edges. Faced with the complexity of gas–solid reactions involving several phases, QXAS in combination with multivariate data analysis enabled us to follow the sulfidation and oxidative regeneration kinetics of both materials, with a description of the evolution of several intermediate phases. Both Mo and Zn K-edge spectroscopic data were analyzed and comparison of the evolution of ternary oxides containing the two elements proved to be an effective way for validating the results.