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用于气相CO转化的钾促进镍基催化剂:催化剂设计与过程建模验证

K-Promoted Ni-Based Catalysts for Gas-Phase CO Conversion: Catalysts Design and Process Modelling Validation.

作者信息

Gandara-Loe J, Portillo E, Odriozola J A, Reina T R, Pastor-Pérez L

机构信息

Department of Inorganic Chemistry and Materials Sciences Institute, University of Seville-CSIC, Seville, Spain.

Chemical and Environmental Engineering Department, School of Engineering, University of Seville, Sevilla, Spain.

出版信息

Front Chem. 2021 Nov 18;9:785571. doi: 10.3389/fchem.2021.785571. eCollection 2021.

Abstract

The exponential growth of greenhouse gas emissions and their associated climate change problems have motivated the development of strategies to reduce CO levels via CO capture and conversion. Reverse water gas shift (RWGS) reaction has been targeted as a promising pathway to convert CO into syngas which is the primary reactive in several reactions to obtain high-value chemicals. Among the different catalysts reported for RWGS, the nickel-based catalyst has been proposed as an alternative to the expensive noble metal catalyst. However, Ni-based catalysts tend to be less active in RWGS reaction conditions due to preference to CO methanation reaction and to the sintering and coke formation. Due to this, the aim of this work is to study the effect of the potassium (K) in Ni/CeO catalyst seeking the optimal catalyst for low-temperature RWGS reaction. We synthesised Ni-based catalyst with different amounts of K:Ni ratio (0.5:10, 1:10, and 2:10) and fully characterised using different physicochemical techniques where was observed the modification on the surface characteristics as a function of the amount of K. Furthermore, it was observed an improvement in the CO selectivity at a lower temperature as a result of the K-Ni-support interactions but also a decrease on the CO conversion. The 1K catalyst presented the best compromise between CO conversion, suppression of CO methanation and enhancing CO selectivity. Finally, the experimental results were contrasted with the trends obtained from the thermodynamics process modelling observing that the result follows in good agreement with the modelling trends giving evidence of the promising behaviour of the designed catalysts in CO high-scale units.

摘要

温室气体排放的指数增长及其相关的气候变化问题推动了通过二氧化碳捕获和转化来降低一氧化碳水平的策略的发展。逆水煤气变换(RWGS)反应已成为将一氧化碳转化为合成气的一条有前景的途径,合成气是几种反应中获得高价值化学品的主要反应物。在报道的用于RWGS的不同催化剂中,镍基催化剂已被提议作为昂贵的贵金属催化剂的替代品。然而,由于倾向于一氧化碳甲烷化反应以及烧结和积炭的形成,镍基催化剂在RWGS反应条件下往往活性较低。因此,本工作的目的是研究钾(K)在镍/氧化铈催化剂中的作用,以寻找用于低温RWGS反应的最佳催化剂。我们合成了不同钾与镍比例(0.5:10、1:10和2:10)的镍基催化剂,并使用不同的物理化学技术进行了全面表征,观察到表面特性随钾含量的变化而改变。此外,由于钾 - 镍 - 载体相互作用,在较低温度下一氧化碳选择性有所提高,但一氧化碳转化率有所下降。1K催化剂在一氧化碳转化率、抑制一氧化碳甲烷化和提高一氧化碳选择性之间表现出最佳的平衡。最后,将实验结果与热力学过程建模得到的趋势进行对比,发现结果与建模趋势吻合良好,这证明了所设计的催化剂在大规模一氧化碳装置中具有良好的应用前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6898/8636742/99085a9c5f5d/fchem-09-785571-g001.jpg

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