In order to reduce CO₂ emissions, it is necessary to substitute fossil fuels with renewable energy using CO₂ as a carbon feedstock. An attractive route for synthetic fuel production is the Fe- or Co-catalysed Fischer–Tropsch process. A profound knowledge of the catalyst deactivation phenomena under industrial conditions is crucial for the process optimisation. In this study, we followed the structural changes of a Co–Ni–Re/γ-Al₂O₃ catalyst for >300 hours at 30 bar and 250 °C during the Fischer–Tropsch synthesis operando at a synchrotron radiation facility. The advanced setup built for operando X-ray diffraction and X-ray absorption spectroscopy allows simultaneous and robust monitoring of the catalytic activity even over 300 h time on stream. We found three activity regimes for the Co–Ni–Re/γ-Al₂O₃ catalyst during 310 h of operation. Fast decline in activity was observed during the initiation phase in the first hours of operation due to liquid film formation (mass transport limitations). Furthermore, solid state reactions and carbon depositions were found while continuing the exposure of the catalyst to harsh temperature conditions of 250 °C. By using this advanced setup, we bridged the gap between industrially oriented catalysts and fundamental studies at synchrotron radiation facilities, opening up new possibilities for operando characterisation of industrial processes that rely on conditions of up to 450 °C and 50 bar.

中文翻译：

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弥合工业与同步加速器之间的鸿沟：费托合成过程中300小时内30 bar进行的操作研究

为了减少CO ₂排放，有必要使用CO ₂作为碳原料，用可再生能源替代化石燃料。Fe或Co催化的Fischer-Tropsch工艺是合成燃料生产的一种有吸引力的途径。对工业条件下催化剂失活现象的深刻了解对于工艺优化至关重要。在这项研究中，我们遵循一个Co-Ni基的Re /γ-Al的结构变化₂ ö ₃催化剂>300小时在30巴和250℃的费-托合成过程中operando在同步加速器辐射设施。专为操作而构建的高级设置X射线衍射和X射线吸收光谱技术可同时且稳定地监控催化活性，即使在运行300小时以上。我们发现有活性的机制为Co-Ni基的Re /γ-Al系₂ ö ₃操作的310小时内催化剂。由于液膜的形成（传质限制），在操作的最初几个小时内，在启动阶段观察到活性迅速下降。此外，发现了固态反应和碳沉积，同时继续将催化剂暴露于250°C的苛刻温度条件下。通过使用这种先进的设置，我们弥合了同步加速器辐射设施中工业导向型催化剂与基础研究之间的鸿沟，为操作性开辟了新的可能性 取决于最高450°C和50 bar的条件的工业过程的表征。