1. Ni-Mn catalysts on silica-modified alumina for CO2 methanation.
- Author
-
Vrijburg, Wilbert L., Garbarino, Gabriella, Chen, Wei, Parastaev, Alexander, Longo, Alessandro, Pidko, Evgeny A., and Hensen, Emiel J.M.
- Subjects
- *
METHANATION , *MIXED oxide catalysts , *CATALYSTS , *CATALYST supports , *X-ray absorption , *ALUMINUM oxide - Abstract
• Mn-promoted Ni catalysts on silica-modified alumina (SA) prepared. • Increasing Mn/Ni ratio yields more active and stable methanation catalysts. • Ni/SA methanation performance promoted by MnO at 1 bar and 20 bar. • Mn addition improves Ni reducibility and dispersion, CO 2 adsorption and activation. • Mn present as MnO clusters on Ni active phase in reduced catalysts. The viability of the Power-to-Gas (PtG) concept is strongly dependent on the development of highly active and stable methanation catalysts obtained from cheap and abundant elements. In this paper, the promotional effect of MnO on Ni catalysts supported on silica-modified γ-Al 2 O 3 (SA) was investigated in CO 2 and CO methanation on catalysts with Mn/Ni atomic ratios between 0 and 0.25. Significantly higher methanation rates and CH 4 selectivities were obtained for Mn-promoted compositions compared to Ni-only catalysts. The optimal NiMn/SA (Mn/Ni = 0.25) catalyst exhibited improved stability compared with unpromoted Ni/SA at 20 bar. The nature of the catalyst precursor and active catalyst was studied with STEM-EDX, XPS, and X-ray absorption spectroscopy (XAS). Evidence of a mixed Ni-Mn oxide in the catalyst precursor was obtained by EXAFS. EXAFS measurements revealed that the reduced catalyst consisted of metallic Ni particles and small oxidic Mn2+ species. Moreover, Mn addition improved the Ni dispersion and enhanced the Ni2+ reducibility by weakening the interaction between the Ni-oxide precursor and the support. A mechanistic study involving IR spectroscopy and steady-state isotopic (13CO 2) transient kinetic analysis (SSITKA) showed that the presence of Mn enhanced CO 2 adsorption and activation. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF