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Multifunctional Catalyst Combination for the Direct Conversion of CO2 to Propane
JACS Au Pub Date : 2021-09-02 , DOI: 10.1021/jacsau.1c00302
Adrian Ramirez 1 , Pierfrancesco Ticali 2 , Davide Salusso 2 , Tomas Cordero-Lanzac 3 , Samy Ould-Chikh 1 , Christian Ahoba-Sam 3 , Aram L Bugaev 4 , Elisa Borfecchia 2 , Sara Morandi 2 , Matteo Signorile 2 , Silvia Bordiga 2 , Jorge Gascon 1 , Unni Olsbye 3
Affiliation  

The production of carbon-rich hydrocarbons via CO2 valorization is essential for the transition to renewable, non-fossil-fuel-based energy sources. However, most of the recent works in the state of the art are devoted to the formation of olefins and aromatics, ignoring the rest of the hydrocarbon commodities that, like propane, are essential to our economy. Hence, in this work, we have developed a highly active and selective PdZn/ZrO2+SAPO-34 multifunctional catalyst for the direct conversion of CO2 to propane. Our multifunctional system displays a total selectivity to propane higher than 50% (with 20% CO, 6% C1, 13% C2, 10% C4, and 1% C5) and a CO2 conversion close to 40% at 350 °C, 50 bar, and 1500 mL g–1 h–1. We attribute these results to the synergy between the intimately mixed PdZn/ZrO2 and SAPO-34 components that shifts the overall reaction equilibrium, boosting CO2 conversion and minimizing CO selectivity. Comparison to a PdZn/ZrO2+ZSM-5 system showed that propane selectivity is further boosted by the topology of SAPO-34. The presence of Pd in the catalyst drives paraffin production via hydrogenation, with more than 99.9% of the products being saturated hydrocarbons, offering very important advantages for the purification of the products.

中文翻译:

用于将 CO2 直接转化为丙烷的多功能催化剂组合

通过 CO 2增值生产富含碳的碳氢化合物对于向可再生、非化石燃料为基础的能源过渡至关重要。然而,最近的大多数最新工作都致力于烯烃和芳烃的形成,而忽略了对我们的经济至关重要的其他碳氢化合物商品,如丙烷。因此,在这项工作中,我们开发了一种高活性和选择性的 PdZn/ZrO 2 +SAPO-34 多功能催化剂,用于将 CO 2直接转化为丙烷。我们的多功能系统对丙烷的总选择性高于 50%(含 20% CO、6% C 1、13% C 2、10% C 4和 1% C 5)和 CO2在 350 °C、50 bar 和 1500 mL g –1 h –1下,转化率接近 40% 。我们将这些结果归因于紧密混合的 PdZn/ZrO 2和 SAPO-34 组分之间的协同作用,它们改变了整体反应平衡,提高了 CO 2转化率并最大限度地降低了 CO 选择性。与 PdZn/ZrO 2 +ZSM-5 系统的比较表明,SAPO-34 的拓扑结构进一步提高了丙烷的选择性。催化剂中钯的存在推动了石蜡的加氢生产,99.9%以上的产物为饱和烃,为产物的提纯提供了非常重要的优势。
更新日期:2021-10-25
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