钙钛矿型复合氧化物负载钴催化剂用于乙醇氧化重整制氢的研究
Perovskite oxides supported cobalt catalysts for oxidation reforming of ethanol to produce hydrogen
采用柠檬酸络合法制备了La1-xCaxFe1-xCoxO3(x=0.3,0.5)钙钛矿复合氧化物催化剂并将其应用于乙醇水蒸汽重整(SRE)和氧化重整(OSRE)制氢反应。采用TPR、XRD、TEM、热重分析手段对催化剂进行了表征。实验结果显示该催化剂具有优良的稳定性和H2选择性。这可是由于钙钛矿中的Co离子在还原气氛下被还原成纳米金属Co并高分散在载体表面,同时纳米金属Co在氧化气氛下又能重新回到钙钛矿晶格中,对使用过的催化剂氧化后也能回到钙钛矿晶格中。在OSRE反应中,正是由于钴物种发生了纳米金属钴与钴离子的循环,因此该催化剂表现出了优良的稳定性和抗积碳性能。
La1-xCaxFe1-xCoxO3 (x=0.3, 0.5) perovskite-type oxide catalysts prepared by citric acid method were used for the steam reforming of ethanol (SRE) and oxidative steam reforming of ethanol (OSRE) to produce hydrogen. The anti-sintering and anti-coking properties of the catalysts for these two reactions have been investigated. The catalysts were characterized by temperature programmed reduction, X-ray diffraction , X-Ray photoelectron spectroscopy, transmission electron microscopy and thermal analysis techniques. The results indicated that the catalyst was highly selective to hydrogen, as well as very stable for OSRE reaction. The cobalt ions in the perovskite structure could be reduced to nanoparticles of metallic cobalt under the reduction atmosphere; the nano metallic cobalt could be oxidized and went back into the lattice of the perovskite structure under the oxidation atmosphere. The nanoparticles of metallic cobalt on the used catalyst could also be oxidized back into the perovskite structure. In the reaction process of OSRE, the cobalt species was possibly cycling as nanoparticles of metallic cobalt and cobalt ions in the perovskite structure, leading to its high anti-sintering stability.
刘源、王自军
氢能、氢能利用化学电化学工业
乙醇氧化重整钴钙钛矿复合氧化物氧空位积碳
oxidative steam reforming of ethanolcobaltperovskite type oxidecarbon depositionsintering
刘源,王自军.钙钛矿型复合氧化物负载钴催化剂用于乙醇氧化重整制氢的研究[EB/OL].(2013-06-28)[2025-08-25].http://www.paper.edu.cn/releasepaper/content/201306-306.点此复制
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