Fe/SAPO-34催化剂制备及其CO加氢制低碳烯烃性能研究

Preparation of Fe/SAPO-34 catalyst and its performance in CO hydrogenation to light olefins

  • 摘要: 费托合成是合成气制低碳烯烃的重要途径,但目前存在产物选择性难以控制、碳效低等问题。本工作采用负压浸渍法制备了一系列不同Fe含量的Fe/SAPO-34催化剂,并评价了其CO加氢反应性能。结合N2吸附-脱附、XRD、SEM、NH3-TPD和CO-TPD等表征手段,揭示了不同Fe含量Fe/SAPO-34催化剂的构效关系。结果表明,随着Fe负载量的增加,催化剂表面酸强度和酸量依次降低,CO的非解离活化能力减弱,CO的解离活化能力增强,从而使低碳烯烃和含氧化合物选择性分别呈现升高和下降的变化趋势。在200 ℃, 2.0 MPa, GHSV=3300 h−1的温和反应条件下,在包含CO2的全碳产物分布中,当铁负载量为5%时,低碳烯烃选择性为16.2%,含氧化合物选择性为52.6%;当铁负载量为25%时,低碳烯烃选择性为31.9%,含氧化合物选择性为16.9%。结合in situ IR表征,提出了催化剂上合理的CO加氢反应机制。本研究为高碳效制低碳烯烃催化剂的研制提供了一条新的路径,展现出良好的应用前景。

     

    Abstract: Fischer-Tropsch synthesis is an important route to synthesize light olefins from syngas. However, precise control of the product selectivity and enhancing carbon utilization efficiency are still challenging. Herein, we prepared a series of Fe/SAPO-34 catalysts with different Fe contents using negative pressure impregnation method, and evaluated their performance in the CO hydrogenation reaction. Combined N2 adsorption/desorption, XRD, SEM, NH3-TPD, and CO-TPD characterizations, the structure−performance relationships of the Fe/SAPO-34 catalysts were clarified. It is found that with the increase of Fe loading, the strength and quantity of the acidity of the catalysts decreased sequentially, while the CO non-dissociation activation ability weakened and the CO dissociation activation ability increased, resulting in an increasing and decreasing trend in the selectivity of light olefins and oxygenates, respectively. Under a mild reaction conditions of 200 ℃, 2.0 MPa, GHSV=3300 h−1, in the carbon products including CO2, the selectivity of light olefins and oxygenates of the 5%Fe/SAPO-34 catalyst is 16.2% and 52.6%, respectively; while that of 25%Fe/SAPO-34 catalyst is 31.9% and 16.9%, respectively. A reasonable reaction mechanism is proposed based on the in situ IR characterization. This study provides a new way for the research and development of the catalyst for light olefins synthesis with enhanced carbon utilization efficiency, showing good application prospects.

     

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