Co-Mn catalysts for H2 production via methane pyrolysis in molten salts

Autor: Sumathy Raman, Joshua J. Willis, Brett Parkinson, Clemens F. Patzschke, Partha Nandi, Klaus Hellgardt, Alyssa M. Love
Rok vydání: 2021
Předmět:
Zdroj: Chemical Engineering Journal. 414:128730
ISSN: 1385-8947
DOI: 10.1016/j.cej.2021.128730
Popis: A promising production route for near CO2-free H2 from natural gas is methane pyrolysis in molten salts. During a screening of catalysts (containing La, Ni, Co and Mn) as particle suspensions in molten NaBr-KBr at 850 °C – 1000 °C, mixed Co-Mn catalysts were identified as being highly promising owing to their stability at pyrolysis conditions and fast kinetics. The catalysts, which contained Co-Mn nanocrystals (~8–9 ± 1 nm) that were prepared by colloidal chemistry were further tested in-depth, and their performance with varying molar Co:Mn ratios, particle sizes and temperatures were examined. The increase of the molar Co:Mn ratio from zero to two increased the CH4 conversion at 1000 °C from 4.8% to 10.4% for the smallest catalyst size range. Furthermore, we observed for all tested Co-Mn catalysts a stable performance over ca. 24 h of methane pyrolysis at 1000 °C and product selectivities for H2 near unity. While the Co-lean particles coked, the surface of the Co-rich particles remained largely carbon-free, and an increase in the Co-content was found to inhibit interactions between the support and the active phase (e.g. inhibited CoAl2O4 and MnAl2O4 formation). The rigorous procedure for the catalyst testing presented in this work enables the field to further investigate the use of catalysts for this process, and the insights gained from experiments with particle suspensions can be applied to the design of structured packings for an industrial-scale process.
Databáze: OpenAIRE