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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >DRIFTS/MS Studies during Chemical Transients and SSITKA of the CO/H2 Reaction over Co-MgO Catalysts
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DRIFTS/MS Studies during Chemical Transients and SSITKA of the CO/H2 Reaction over Co-MgO Catalysts

机译：Co-MgO催化剂上化学瞬变过程中的DRIFTS / MS研究和CO / H2反应的SSITKA

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摘要

Diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) has been employed along with chemical and isotope transients to study the catalytic CO hydrogenation over Co/MgO catalysts in a single fixed-bed reactor at T = 523 K and ambient pressure conditions (H2/CO = 3). According to the operando DRIFTS measurements, the catalyst surface contains hydroxyl groups, adsorbed CO, formate, and methylene groups in the steady-state of the reaction. Transient experiments following fast changes in the feed (chemical transient kinetics, CTK) or isotope composition (steady-state isotopic transient kinetic analysis, SSITKA) have been carried out during DRIFTS and demonstrate that the formate/methylene "seen by DRIFTS" plays no role as imminent intermediates of the ambient pressure Fischer-Tropsch (FT) reaction. The SSITKA experiments (replacing ~(12)CO by ~(13)CO) show that the exchange rate of formate/methylene is significantly lower than that of ethane, which is one of the main reaction products of CO hydrogenation (followed by mass spectrometry). Formate is most probably bound as bidentate μ2-species to MgO or at the Co/MgO interface, while methylene stands for skeleton CH2 in either hydrocarbon or carboxylate.
机译：扩散反射傅里叶变换红外光谱（DRIFTS）已与化学和同位素瞬变一起用于研究在固定床反应器中T / 523 K和环境压力条件（H2 / CO = 3）。根据操作DRIFTS测量，在反应的稳态下，催化剂表面包含羟基，吸附的CO，甲酸酯和亚甲基。在DRIFTS期间进行了进料（化学瞬态动力学，CTK）或同位素组成（稳态同位素瞬态动力学分析，SSITKA）快速变化的瞬态实验，结果表明“ DRIFTS所见”的甲酸酯/亚甲基没有作用作为环境压力即将发生的费托（FT）反应的中间体。 SSITKA实验（用〜（13）CO代替〜（12）CO）表明甲酸/亚甲基的交换速率明显低于乙烷，后者是CO加氢的主要反应产物之一（随后是质谱） ）。甲酸酯最有可能作为M2O或Co / MgO界面的二齿μ2物种键合，而亚甲基则代表烃或羧酸酯中的骨架CH2。

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