Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.
Faculty of Physics and CENIDE, Universität Duisburg-Essen, Forsthausweg 2, Duisburg, Germany.
Angew Chem Int Ed Engl. 2017 Sep 11;56(38):11480-11484. doi: 10.1002/anie.201705714. Epub 2017 Aug 15.
Tandem catalysis is an attractive strategy to intensify chemical technologies. However, simultaneous control over the individual and concerted catalyst performances poses a challenge. We demonstrate that enhanced pore transport within a Co/Al O Fischer-Tropsch (FT) catalyst with hierarchical porosity enables its tandem integration with a Pt/ZSM-5 zeolitic hydrotreating catalyst in a spatially distant fashion that allows for catalyst-specific temperature adjustment. Nevertheless, this system resembles the case of close active-site proximity by mitigating secondary reactions of primary FT α-olefin products. This approach enables the combination of in situ dewaxing with a minimum production of gaseous hydrocarbons (18 wt %) and an up to twofold higher (50 wt %) selectivity to middle distillates compared to tandem pairs based on benchmark mesoporous FT catalysts. An overall 80 % selectivity to liquid hydrocarbons from syngas is attained in one step, attesting to the potential of this strategy for increasing the carbon efficiency in intensified gas-to-liquid technologies.
串联催化是强化化学技术的一种有吸引力的策略。然而,同时控制单个和协同催化剂的性能是一个挑战。我们证明了在具有分级孔结构的 Co/Al2O3费托(FT)催化剂内增强孔传输能力,可以将其与 Pt/ZSM-5沸石加氢处理催化剂以空间上的远程方式串联集成,从而允许对催化剂进行特定温度的调节。然而,通过减轻初级 FTα-烯烃产物的次要反应,该系统类似于活性位近距离的情况。这种方法能够将原位脱蜡与最小化气态烃(18wt%)的生产相结合,并与基于基准介孔 FT 催化剂的串联对相比,选择性提高一倍(50wt%)至中间馏分。一步法从合成气中获得了 80%的液体烃总选择性,证明了这种策略在提高强化气-液技术中的碳效率方面的潜力。