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共进料水对用原子层沉积或分子层沉积包覆层改性的Co-Pt-Si/γ-AlO费托合成催化剂的影响

Effect of Co-fed Water on a Co-Pt-Si/γ-AlO Fischer-Tropsch Catalyst Modified with an Atomic Layer Deposited or Molecular Layer Deposition Overcoating.

作者信息

Heikkinen Niko, Keskiväli Laura, Palo Jasmiina, Reinikainen Matti, Putkonen Matti

机构信息

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.

出版信息

ACS Omega. 2022 Feb 23;7(9):7725-7736. doi: 10.1021/acsomega.1c06512. eCollection 2022 Mar 8.

Abstract

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.

摘要

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。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1992/8908501/7fb9b7d8c3a7/ao1c06512_0002.jpg

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