E. Kraleva , H. Lund , J. Weiß , S. Bartling , H. Atia , Z. Cherkezova-Zheleva , D. Paneva , S. Wohlrab , U. Armbruster
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引用次数: 0
Abstract
To improve the CO2-to-light olefin process in terms of economics, efficient catalysts are essential to maximize the yield. Our research was carried out on FeAlCuK, which is still considered as a benchmark for olefin formation via CO2 Fischer-Tropsch synthesis (FTS). Nevertheless, the effect of various activation conditions on the formation of desired active species and final activity of this catalyst has not been described in literature to date. We studied the pretreatment by varying both the reduction gas and temperature. The catalyst was pretreated with pure H2 or synthesis gas (H2/CO = 3) to identify the bulk and surface species formed in each case. We demonstrate that the FeCuAlK catalyst should be activated in a H2/CO atmosphere at 250 °C for 4 h before the test at typical FTS reaction conditions to reach maximum productivity. The reduction with H2/CO led to the formation of active Fe5C2 and Fe3O4 phases producing a high fraction of light olefins at higher CO2 conversion. The role of promoters K and Cu was also investigated. Selectivity for desired C2-C4 olefins increased by 10 % compared to catalysts which were used directly in FTS without preliminary activation. Characterization with ex and in situ powder X-ray diffraction, Raman spectroscopy, and XPS after each activation treatment as well as Mössbauer spectroscopy revealed a strong impact of gas nature on the phase composition which was correlated with the performance.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.