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The Effect of Copper Addition on the Activity and Stability of Iron-Based CO2 Hydrogenation Catalysts

机译:铜添加对铁基CO2加氢催化剂活性和稳定性的影响

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摘要

Iron-based CO2 catalysts have shown promise as a viable route to the production of olefins from CO2 and H2 gas. However, these catalysts can suffer from low conversion and high methane selectivity, as well as being particularly vulnerable to water produced during the reaction. In an effort to improve both the activity and durability of iron-based catalysts on an alumina support, copper (10–30%) has been added to the catalyst matrix. In this paper, the effects of copper addition on the catalyst activity and morphology are examined. The addition of 10% copper significantly increases the CO2 conversion, and decreases methane and carbon monoxide selectivity, without significantly altering the crystallinity and structure of the catalyst itself. The FeCu/K catalysts form an inverse spinel crystal phase that is independent of copper content and a metallic phase that increases in abundance with copper loading (>10% Cu). At higher loadings, copper separates from the iron oxide phase and produces metallic copper as shown by SEM-EDS. An addition of copper appears to increase the rate of the Fischer–Tropsch reaction step, as shown by modeling of the chemical kinetics and the inter- and intra-particle transport of mass and energy.
机译:铁基CO2催化剂显示出有望成为从CO2和H2气体生产烯烃的可行途径。然而,这些催化剂可能具有低转化率和高甲烷选择性的缺点,并且特别易受反应过程中产生的水的影响。为了提高氧化铝载体上铁基催化剂的活性和耐用性,已将铜(10–30%)添加到催化剂基质中。在本文中,研究了铜添加对催化剂活性和形态的影响。添加10%的铜可显着提高CO2转化率,并降低甲烷和一氧化碳的选择性,而不会显着改变催化剂本身的结晶度和结构。 FeCu / K催化剂形成与铜含量无关的反尖晶石晶体相,以及随铜含量(> 10%Cu)而增加的金属相。如SEM-EDS所示,在较高的负载下,铜会与氧化铁相分离并生成金属铜。化学模型以及质量和能量在颗粒间和颗粒内的传递模型表明,添加铜似乎可以提高费-托反应步骤的速率。

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