过渡金属掺杂对 ZSM-5 沸石催化剂在乙醇-烃转化过程中的性质和催化性能的影响

Ifeanyi Michael Smarte Anekwe , Bilainu Oboirien , Yusuf Makarfi Isa
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摘要

本研究利用实验数据和文献资料研究了过渡金属掺杂对HZSM-5催化剂的理化性质和催化性能的影响。采用不同浓度(0.5 wt%和10 wt%)的过渡金属(Co, Fe, Ni)对水热合成的新型ZSM-5催化剂进行改性。通过x射线衍射、傅里叶变换红外光谱、扫描电镜、能量色散x射线光谱、粒度分布、N2吸附和NH3程序升温脱附等表征,揭示了催化剂性能的变化。过渡金属的引入影响了MFI的表面积、粒径和酸度,但没有改变MFI的结构。特别是,与纯催化剂的表面积(397.5 m²/g)相比,观察到的表面积减少幅度为2.6%至23%,对应于不同的金属负载0.5-10 wt%。此外,金属掺杂导致路易斯酸位点增加,强酸位点减少。在350°C和12 h−1空速下的催化评价表明,与未改性的催化剂相比,金属掺杂的ZSM-5催化剂的性能有所改善,对燃料范围内的碳氢化合物具有较高的选择性。低金属掺杂的催化剂表现出最佳的催化活性,而高金属掺杂导致焦炭沉积增加,催化剂因强酸浓度增加而失活。这些结果强调了金属改性ZSM-5在碳氢化合物反应中的适用性,并为优化乙醇转化为燃料型碳氢化合物的催化剂提供了有价值的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Effects of transition metal doping on the properties and catalytic performance of ZSM-5 zeolite catalyst on ethanol-to-hydrocarbons conversion

In this study, the effects of transition metal-doping on the physicochemical properties and catalytic performance of HZSM-5 catalysts for the conversion of ethanol to hydrocarbons are investigated using experimental data and secondary data from the literature. Hydrothermally synthesized novel ZSM-5 catalysts were modified with different concentrations (0.5 and 10 wt%) of transition metals (Co, Fe, Ni). Characterizations, including X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy, particle size distribution, N2 adsorption and NH3 temperature-programmed desorption, revealed the changes in catalyst properties. The introduction of transition metals affected the surface area, particle size and acidity without altering the MFI structures. In particular, a reduction in surface area was observed, ranging from 2.6 to 23 %, corresponding to the different metal loading of 0.5–10 wt% compared to the surface area of the pure catalyst (397.5 m²/g). In addition, metal-doping led to an increase in Lewis acid sites, accompanied by a decrease in strong acid sites. Catalytic evaluation at 350 °C and a space velocity of 12 h−1 showed improved performance in metal-doped ZSM-5 catalysts, which exhibited high selectivity towards fuel-range hydrocarbons, compared to the unmodified catalyst. Catalysts with low metal doping showed optimal catalytic activity, while high metal doping led to increased coke deposition and deactivation of the catalyst due to an increased concentration of strong acids. These results underline the suitability of metal-modified ZSM-5 for hydrocarbon reactions and provide valuable insights for the optimization of catalysts for ethanol conversion to fuel-range hydrocarbons.

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