Heikkinen Niko, Keskiväli Laura, Palo Jasmiina, Reinikainen Matti, Putkonen Matti
VTT Technical Research Centre of Finland, P.O.Box 1000, FIN-02044 VTT, Espoo, Finland.
Department of Chemistry, University of Helsinki, P.O.Box 55, FIN-00014 Helsinki, Finland.
ACS Omega. 2022 Feb 23;7(9):7725-7736. doi: 10.1021/acsomega.1c06512. eCollection 2022 Mar 8.
Atomic layer deposition (ALD) and molecular layer deposition (MLD) methods were used to prepare overcoatings on a cobalt-based Fischer-Tropsch catalyst. A Co-Pt-Si/γ-AlO catalyst (21.4 wt % Co, 0.2 wt % Pt, and 1.6 wt % Si) prepared by incipient wetness impregnation was ALD overcoated with 30-40 cycles of trimethylaluminum (TMA) and water, followed by temperature treatment (420 °C) in an inert nitrogen atmosphere. MLD-overcoated samples with corresponding film thicknesses were prepared by using TMA and ethylene glycol, followed by temperature treatment (400 °C) in an oxidative synthetic air atmosphere. The ALD catalyst (40 deposition cycles) had a positive activity effect upon moderate water addition ( / = 0.42), and compared with a non-overcoated catalyst, it showed resistance to irreversible deactivation after co-fed water conditions. In addition, MLD overcoatings had a positive effect on the catalyst activity upon moderate water addition. However, compared with a non-overcoated catalyst, only the 10-cycle MLD-overcoated catalyst retained increased activity throughout high added water conditions ( / = 0.71). All catalyst variations exhibited irreversible deactivation under high added water conditions.
采用原子层沉积(ALD)和分子层沉积(MLD)方法在钴基费托催化剂上制备外涂层。通过初湿浸渍法制备的Co-Pt-Si/γ-AlO催化剂(21.4 wt% Co、0.2 wt% Pt和1.6 wt% Si)用三甲基铝(TMA)和水进行30 - 40个循环的ALD外涂层处理,随后在惰性氮气气氛中进行温度处理(420°C)。使用TMA和乙二醇制备具有相应膜厚的MLD外涂层样品,随后在氧化性合成空气气氛中进行温度处理(400°C)。ALD催化剂(40次沉积循环)在适度加水(/ = 0.42)时具有积极的活性效应,并且与未外涂层的催化剂相比,在共进料水条件下显示出对不可逆失活的抗性。此外,MLD外涂层在适度加水时对催化剂活性有积极影响。然而,与未外涂层的催化剂相比,只有10次循环的MLD外涂层催化剂在高加水条件下(/ = 0.71)始终保持活性增加。所有催化剂变体在高加水条件下均表现出不可逆失活。