基于类钙钛矿铁氧体的含镍(Co)乙醇蒸汽重整催化剂

M. Arapova, S. Pavlova, V. Rogov, T. Krieger, A. Ishchenko, A. Roger
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引用次数: 10

摘要

摘要研究了两种铁酸镨系催化剂的结构、氧化还原性能及其在乙醇蒸汽重整中的性能。第一个系列是通过改性Pechini路线制备的PrFe1-xNi(Co)xO3 (x=0.3-0.4)钙钛矿,第二个系列是通过浸渍PrFeO3制备的不同分散度的5%wt. ni (Co)/PrFeO3,包括5%wt改性的样品。在700℃以上的温度下,所有催化剂的主要产物都是氢和CO。在700℃以下的温度下,负载型催化剂的初始乙醇转化率和产氢率都高于含Ni(CO)钙钛矿催化剂。由钙钛矿衍生的ni基催化剂比co基催化剂更有活性,而co负载的PrFeO3钙钛矿的初始活性比ni负载的更高。对废催化剂的长期实验和TEM研究表明,钙钛矿衍生催化剂比钙钛矿负载催化剂具有更高的结焦稳定性,这是由于形成了高度分散的Ni-Fe合金颗粒,与无序的钙钛矿样基质强烈相互作用。Mo负载方式对Ni/PrFeO3基催化剂的初始活性影响较小,但明显改变了其结焦稳定性,连续浸渍法制备的5%Mo/5%Ni/PrFeO3基催化剂的稳定性在钙钛矿负载催化剂中最高。
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Ni(Co)-containing catalysts based on perovskite-like ferrites for steam reforming of ethanol
Abstract For two series of catalysts based on praseodymium ferrite, their structural and redox properties as well as performance in ethanol steam reforming have been studied. The first series was PrFe1-xNi(Co)xO3 (x=0.3-0.4) perovskites prepared by modified Pechini route, and the second one was 5%wt.Ni(Co)/PrFeO3 of different dispersion prepared by impregnation of PrFeO3, including samples modified by 5%wt. Mo. At temperatures above 700°C, for all catalysts, the main products were hydrogen and CO. At temperatures below 700°C, initial ethanol conversion and hydrogen yield were higher for supported catalysts as compared with ones derived from Ni(Co)-containing perovskites. While Ni-based catalysts derived from perovskite were more active as compared with Co-based samples, Co-supported PrFeO3 perovskite has shown a higher initial activity as compared with Ni-supported one. The long-term tests in the realistic feed and TEM studies of spent catalysts revealed that perovskite-derived catalysts have a higher coking stability than perovskite-supported ones due to formation of highly dispersed Ni-Fe alloy particles strongly interacting with disordered perovskite–like matrix. The method of Mo supporting only slightly affects the initial activity of Ni/PrFeO3–based catalysts but noticeably modifies their coking stability: 5%Mo/5%Ni/PrFeO3 catalyst prepared by successive impregnation possesses the highest stability among perovskite-supported catalysts.
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