Perovskite-Type Oxide Catalysts in CO2 Utilization: A Principal Study of Novel Cu-Doped Perovskites for Methanol Synthesis

Compounds Pub Date : 2022-12-14 DOI:10.3390/compounds2040031
F. Schrenk, L. Lindenthal, Gernot Pacholik, Tina Navratil, Tobias Maximilian Berger, H. Drexler, R. Rameshan, T. Ruh, K. Föttinger, C. Rameshan
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Abstract

Six different perovskite-type oxides were investigated with respect to their ability for methanol synthesis via H2 and CO2: Fe-, Mn-, and Ti-based perovskites were prepared with and without Cu doping. For assessment, the catalysts were subjected to preliminary tests at atmospheric pressure to evaluate their ability to activate CO2. Additional catalytic tests with the doped versions of each catalyst type were carried out in a pressured reactor at 21 bar. After the measurements, the catalysts were characterized with X-ray diffraction (XRD) and scanning electron microscopy (SEM). All catalysts were able to produce methanol in the pressure tests. CO2 conversions between 14% and 23% were reached at 400 °C, with the highest methanol selectivity at the lower temperature of 250 °C. The combination of XRD and SEM revealed that the Fe-based and Ti-based perovskites were stable under reaction conditions and that catalytically highly active and stable nanoparticles had formed. The minor formation of CaCO3, which is a deactivating phase, was observed for one catalyst. These nanoparticles showed resistance to coking and sintering. However, the yield and selectivity for methanol need to be improved via the further tailoring of the perovskite composition.
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钙钛矿型氧化物催化剂在CO2利用中的应用:新型cu掺杂钙钛矿甲醇合成的主要研究
研究了6种不同的钙钛矿型氧化物通过H2和CO2合成甲醇的能力:分别制备了Fe基、Mn基和ti基钙钛矿。为了评估,在常压下对催化剂进行了初步测试,以评估其激活CO2的能力。在21巴压力反应器中对每种催化剂类型的掺杂版本进行了额外的催化试验。测定后,用x射线衍射仪(XRD)和扫描电镜(SEM)对催化剂进行了表征。在压力试验中,所有催化剂都能产生甲醇。在400℃时CO2转化率达到14% ~ 23%,在250℃时甲醇选择性最高。XRD和SEM分析表明,fe基和ti基钙钛矿在反应条件下是稳定的,形成了催化活性高且稳定的纳米颗粒。在一种催化剂上观察到少量CaCO3的形成,这是一种失活相。这些纳米颗粒具有抗焦化和烧结的性能。然而,需要通过进一步调整钙钛矿的组成来提高甲醇的收率和选择性。
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