Raman Narayanan, Wolf Moritz, Heller Martina, Heene-Würl Nina, Taccardi Nicola, Haumann Marco, Felfer Peter, Wasserscheid Peter
Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Lehrstuhl für Chemische Reaktionstechnik (CRT), Egerlandstr. 3, 91058 Erlangen, Germany.
Forschungszentrum Jülich GmbH, Helmholtz-Institute Erlangen-Nürnberg for Renewable Energy (IEK-11), Egerlandstr. 3, 91058 Erlangen, Germany.
ACS Catal. 2021 Nov 5;11(21):13423-13433. doi: 10.1021/acscatal.1c01924. Epub 2021 Oct 21.
Supported catalytically active liquid metal solutions (SCALMS) of Pt in Ga (2 at.-% Pt) were studied in the temperature range of 500 to 600 °C for propane dehydrogenation. A facile synthesis procedure using ultrasonication was implemented and compared to a previously reported organo-chemical route for gallium deposition. The procedure was applied to synthesize GaPt-SCALMS catalyst on silica (SiO), alumina (AlO), and silicon carbide (SiC) to investigate the effect of the support material on the catalytic performance. The SiC-based SCALMS catalyst showed the highest activity, while SiO-based SCALMS showed the highest stability and lowest cracking tendency at higher temperatures. The selectivity toward propene for the SiO-based catalyst remained above 93% at 600 °C. The catalysts were analyzed for coke content after use by temperature-programmed oxidation (TPO) and Raman spectroscopy. While the SiC- and SiO-supported SCALMS systems showed hardly any coke formation, the AlO-supported systems suffered from pronounced coking. SEM-EDX analyses of the catalysts before and after reaction indicated that no perceivable morphological changes occur during reaction. The SCALMS catalysts under investigation are compared with supported Pt and supported GaPt solid-phase catalyst, and possible deactivation pathways are discussed.
研究了镓中铂(2原子百分比铂)的负载型催化活性液态金属溶液(SCALMS)在500至600°C温度范围内用于丙烷脱氢的情况。实施了一种使用超声处理的简便合成程序,并与先前报道的用于镓沉积的有机化学路线进行了比较。该程序用于在二氧化硅(SiO)、氧化铝(AlO)和碳化硅(SiC)上合成GaPt-SCALMS催化剂,以研究载体材料对催化性能的影响。基于SiC的SCALMS催化剂表现出最高的活性,而基于SiO的SCALMS在较高温度下表现出最高的稳定性和最低的裂解倾向。在600°C时,基于SiO的催化剂对丙烯的选择性保持在93%以上。使用程序升温氧化(TPO)和拉曼光谱对使用后的催化剂的焦炭含量进行了分析。虽然基于SiC和SiO负载的SCALMS系统几乎没有焦炭形成,但基于AlO负载的系统存在明显的结焦现象。对反应前后催化剂的SEM-EDX分析表明,反应过程中没有可察觉的形态变化。将所研究的SCALMS催化剂与负载型铂和负载型GaPt固相催化剂进行了比较,并讨论了可能的失活途径。