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A comparative study of manganese–cerium doped metal–organic frameworks prepared via impregnation and in situ methods in the selective catalytic reduction of NO

机译:通过 浸渍和原位方法制备的锰铈掺杂金属有机骨架在NO的选择性催化还原中的比较研究

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Mn and Ce were loaded on metal–organic frameworks (MOFs) via impregnation and in situ doping methods. The catalytic capacities of the obtained composite materials were evaluated in the selective catalytic reduction (SCR) of NO. The existing form of Mn–Ce in the MOF originates from different doping methods and its effect on the catalytic performance was investigated. Mn–Ce introduced by impregnation was deposited on the surface of the MOF and exhibited high catalytic efficiency of more than 98% from 200 °C to 300 °C. According to the results of BET, XRD, XPS, and ICP analyses, it was concluded that Mn–Ce introduced via the in situ doping method was inserted in the crystal lattice structure of the MOF, which resulted in an enlarged surface area, low Mn concentration, and poor redox property as compared to that introduced via the impregnated method. By exploring these factors, it was proven that the limited redox ability was the direct reason that resulted in the low activity of the MnCeMOF. Using thermal decomposition, the in situ doped Mn–Ce was liberated from the MnCeMOF crystal lattice and subsequently, exhibited recovered redox properties and catalytic activity. In this study, we proved that different doping methods lead to different forms of Mn–Ce in the MOF, which exhibit different redox properties and thus directly lead to different catalytic performance.
机译:通过浸渍和原位掺杂方法将锰和铈加载到金属有机骨架(MOF)上。通过NO的选择性催化还原(SCR)来评估所获得的复合材料的催化能力。 MOF中Mn-Ce的现有形式源自不同的掺杂方法,并研究了其对催化性能的影响。通过浸渍引入的Mn–Ce沉积在MOF的表面上,并且从200°C到300°C表现出98%以上的高催化效率。根据BET,XRD,XPS和ICP分析的结果,可以得出结论,将通过原位掺杂方法引入的Mn-Ce插入了晶格结构。与通过浸渍法引入的相比,MOF具有更大的表面积,较低的Mn浓度和较差的氧化还原性能。通过探索这些因素,证明了有限的氧化还原能力是导致MnCeMOF活性低的直接原因。通过热分解,从MnCeMOF晶格中释放出原位掺杂的Mn-Ce,随后表现出恢复的氧化还原特性和催化活性。在这项研究中,我们证明了不同的掺杂方法会在MOF中导致不同形式的Mn–Ce,表现出不同的氧化还原特性,从而直接导致不同的催化性能。

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