Merkouri Loukia-Pantzechroula, Ramirez Reina Tomas, Duyar Melis S
Department of Chemical and Process Engineering, University of Surrey, Guildford, GU2 7XH UK.
Department of Inorganic Chemistry and Materials Sciences Institute, University of Seville-CSIC, 41092, Seville, Spain.
Nanoscale. 2022 Sep 15;14(35):12620-12637. doi: 10.1039/d2nr02688k.
The feasibility of a Dual Function Material (DFM) with a versatile catalyst offering switchable chemical synthesis from carbon dioxide (CO) was demonstrated for the first time, showing evidence of the ability of these DFMs to passively capture CO directly from the air as well. These DFMs open up possibilities in flexible chemical production from dilute sources of CO, through a combination of CO adsorption and subsequent chemical transformation (methanation, reverse water gas shift or dry reforming of methane). Combinations of Ni Ru bimetallic catalyst with NaO, KO or CaO adsorbent were supported on CeO-AlO to develop flexible DFMs. The designed multicomponent materials were shown to reversibly adsorb CO between the 350 and 650 °C temperature range and were easily regenerated by an inert gas purge stream. The components of the flexible DFMs showed a high degree of interaction with each other, which evidently enhanced their CO capture performance ranging from 0.14 to 0.49 mol kg. It was shown that captured CO could be converted into useful products through either CO methanation, reverse water-gas shift (RWGS) or dry reforming of methane (DRM), which provides flexibility in terms of co-reactant (hydrogen . methane) and end product (synthetic natural gas, syngas or CO) by adjusting reaction conditions. The best DFM was the one containing CaO, producing 104 μmol of CH per kg in CO methanation, 58 μmol of CO per kg in RWGS and 338 μmol of CO per kg in DRM.
首次证明了具有多功能催化剂的双功能材料(DFM)实现从二氧化碳(CO)进行可切换化学合成的可行性,这也表明这些DFM具备直接从空气中被动捕获CO的能力。通过CO吸附及随后的化学转化(甲烷化、逆水煤气变换或甲烷干重整)相结合,这些DFM为从稀CO源进行灵活的化学生产开辟了可能性。将Ni Ru双金属催化剂与NaO、KO或CaO吸附剂的组合负载在CeO - AlO上,以开发灵活的DFM。所设计的多组分材料在350至650°C温度范围内可逆地吸附CO,并通过惰性气体吹扫流轻松再生。灵活DFM的各组分之间表现出高度的相互作用,这明显提高了它们的CO捕获性能,范围为0.14至0.49 mol/kg。结果表明,捕获的CO可通过CO甲烷化、逆水煤气变换(RWGS)或甲烷干重整(DRM)转化为有用的产物,通过调整反应条件,在共反应物(氢气、甲烷)和最终产物(合成天然气、合成气或CO)方面提供了灵活性。最佳的DFM是含有CaO的DFM,在CO甲烷化中每千克产生104 μmol的CH,在RWGS中每千克产生58 μmol的CO,在DRM中每千克产生338 μmol的CO。