Structure–Activity Relationships of Copper- and Potassium-Modified Iron Oxide Catalysts during Reverse Water–Gas Shift Reaction,ACS Catalysis

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Structure–Activity Relationships of Copper- and Potassium-Modified Iron Oxide Catalysts during Reverse Water–Gas Shift Reaction
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-09-30 , DOI: 10.1021/acscatal.1c03792
Mengwei Gu ₁ , Sheng Dai ₂ , Runfa Qiu ₁ , Michael E. Ford ₃ , Chenxi Cao ₄ , Israel E. Wachs ₃ , Minghui Zhu ₁

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The reverse water–gas shift (RWGS) reaction is an initial and essential step for CO₂ hydrogenation. In this study, Cu- and K-modified iron oxide catalysts were investigated with a series of in/ex-situ characterization techniques, including in situ XRD, in situ Raman, in situ DRIFTS quasi in situ XPS, quasi in situ HS-LEIS, H₂-TPR, CO₂-TPD, and TPSR. The surface structure of the catalyst is found to strongly depend on the presence of Cu and K, leading to diverse reducibility and basicity. Adding K to the iron-based catalyst alters the reaction from a redox pathway that proceeds on surface redox sites to an associative pathway that proceeds on surface redox and basic sites. Metallic Cu facilitates hydrogen dissociation and promotes both mechanisms by either boosting surface vacancy sites or supplying abundant surface hydrogen atoms. These findings would be beneficial for the rational design of CO₂ hydrogenation catalysts.

中文翻译：

铜和钾改性氧化铁催化剂在逆向水煤气变换反应中的构效关系

逆水煤气变换 (RWGS) 反应是 CO ₂加氢的初始且必不可少的步骤。在这项研究中，使用一系列原位/非原位表征技术研究了 Cu 和 K 改性的氧化铁催化剂，包括原位XRD、原位拉曼、原位DRIFTS 准原位XPS、准原位HS-LEIS , H ₂ -TPR, CO ₂-TPD 和 TPSR。发现催化剂的表面结构强烈依赖于 Cu 和 K 的存在，导致不同的还原性和碱性。向铁基催化剂中添加 K 可将反应从在表面氧化还原位点上进行的氧化还原途径改变为在表面氧化还原和碱性位点上进行的缔合途径。金属铜通过增加表面空位或提供丰富的表面氢原子来促进氢离解并促进这两种机制。这些发现将有利于CO ₂加氢催化剂的合理设计。

更新日期：2021-10-15

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