Ln(Ln = La,Pr,Nd,Sm)对含钙双相膜结构和透氧性能的影响
Influence of Ln elements (Ln = La, Pr, Nd, Sm) on the structure and oxygen permeability of Ca-containing dual-phase membranes
摘要:
基于氧燃料概念开发用于CO2捕获的良好性能和低成本的氧可渗透膜是非常期望的,但具有挑战性。尽管在探索新的CO2稳定的双相膜方面做出了巨大努力,但其存在仍然远远不能满足工业要求。本文报道了一系列新的含钙耐CO2氧传输膜,其组成为60 wt.% Ce0.9Ln0.1O2-40wt.%通过Pechini一锅法合成了Ln0.6Ca0.4FeO3(CLnO-LnCFO; Ln = La,Pr,Nd,Sm)。结果表明,所研究的化合物均由钙钛矿相和萤石相组成,而hoc-NCFO和CSO-SCFO膜中的钙钛矿相在烧结后分别生成了富钙和贫钙两种不同形貌的晶粒,其中贫钙的小钙钛矿晶粒阻碍了氧离子的传输,最终导致透氧性能变差。在我们研究的CLnO-LnCFO膜中,CPO-PCFO具有最高的透氧性和优异的CO2稳定性,这主要与晶体对称性的改善、不可忽略的萤石相的电子电导率和钙钛矿的电子电导率的增强有关。我们的研究结果建立了含钙氧化物作为候选材料平台的膜工程设备,结合二氧化碳捕获和氧气分离。
英文摘要:
Developing good performance and low-cost oxygen permeable membranes for CO2 capture based on the oxy-fuel concept is greatly desirable but challenging. Despite tremendous efforts in exploring new CO2-stable dual-phase membranes, its presence is however still far from meeting the industrial requirements. Here we report a series of new Ca-containing CO2-resistant oxygen transporting membranes with composition 60wt.%Ce0.9Ln0.1O2-40wt.%Ln0.6Ca0.4FeO3(CLnO-LnCFO; Ln = La, Pr, Nd, Sm) synthesized via a Pechini one-pot method. Our results indicate all investigated compounds are composed of perovskite and fluorite phases, while the perovskite phases in the CNO-NCFO and CSO-SCFO membranes after sintering generates Ca-rich and Ca-less two kinds of grains with different morphologies, where the Ca-less small perovskite grains block the transport of oxygen ions and eventually result in poor oxygen permeability. Among our investigated CLnO-LnCFO membranes, CPO-PCFO exhibits the highest oxygen permeability and excellent CO2 stability, which were mainly associated with the improvement in crystal symmetry, non-negligible electronic conductivity of fluorite phase and the enhancement in electronic conductivity of perovskite. Our results establish Ca-containing oxides as candidate material platforms for membrane engineering devices that combine CO2 capture and oxygen separation.
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