Herein, we provide fundamentals relevant for the development of Fe-based catalysts for CO2hydrogenation to higher hydrocarbons. It was possible owing to preparation of well-defined FexOyCz compositions through controlled decomposition of iron oxalate, determination of their composition under CO2-FT reaction and catalytic tests in a broad range of CO2 conversion. Such steady-state composition changes along the catalyst bed. The changes and their strength depend on the initial phase composition. In addition to the reaction-induced catalyst restructuring, reaction pathways leading from CO2 to CO, CH4 and higher hydrocarbons were elucidated. A correlation between them and the steady-state composition was established and offers the possibility for tailored catalyst design and preparation. Our best performing promoter-free Fe-based catalyst shows the selectivity to CH4 below 10 %, while the selectivity to C2+-hydrocarbons is about 50 % at CO2 conversion of about 25 % and 300 °C. The olefin to paraffin ratio among C2-C4 hydrocarbons is 5.5.
Предметные области OECD FOS+WOS
- 2.04 ХИМИЧЕСКИЕ ТЕХНОЛОГИИ
- 1.05 НАУКИ О ЗЕМЛЕ И СМЕЖНЫЕ ЭКОЛОГИЧЕСКИЕ НАУКИ