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Iron precipitated onto ceria-zirconia nanoparticle mixtures for the production of hydrogen via two-step thermochemical water splitting
International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2018-06-19 , DOI: 10.1016/j.ijhydene.2018.05.043
Samantha J. Roberts , Nathan G. Carr , Jonathan McLaughlin , Helena E. Hagelin-Weaver

Several novel materials were synthesized by precipitating iron oxide (using the previously optimized 10% Fe loading by weight) onto mixtures of nanoparticle zirconia and ceria to investigate the effects of adding CeO2 to FeOx/ZrO2 materials in the thermochemical water splitting reaction. At water splitting temperatures of 1000 °C (after thermal reduction at 1450 °C), the stability of the CeO2-containing materials was lower than for the FeOx/ZrO2 material, and there was no advantage to adding CeO2 to the FeOx/ZrO2 material. However, when operating at a water splitting (WS) temperature of 1200 °C, the stability increased and the hydrogen production was significantly higher over most materials compared with a water splitting temperature of 1000 °C. At a WS temperature of 1200 °C the FeOx/Zr75Ce25O2 (75% Zr75O2 and 25% CeO2 by weight) and FeOx/Zr50Ce50O2 materials performed slightly better than the FeOx/ZrO2 material, and X-ray photoelectron spectroscopy data revealed that the surface concertation of iron is less important compared with water splitting at 1000 °C. The temperature programmed reduction data indicated that the FeOx-CeO2 interactions were weaker compared with FeOx-ZrO2 interactions, since the FeOx reduction occurred at lower temperatures for the CeO2-containing materials. The weaker interactions can explain why the stability was lower for the materials containing CeO2 (sintering of FeOx was likely more pronounced) The X-ray diffraction data revealed that ZrO2-CeO2 solid solutions formed after activation at 1450 °C and lattice volume calculations indicated that iron did incorporate into the ZrO2-CeO2 matrices. More incorporation was observed after water-splitting at 1200 °C compared with a lower temperature (1000 °C), and likely explains why the materials were more stable during water-splitting at 1200 °C.



中文翻译:

铁沉淀在二氧化铈-氧化锆纳米颗粒混合物上,用于通过两步热化学水分解制氢

通过将氧化铁沉淀(使用先前优化的10%重量的Fe负载)到纳米氧化锆和二氧化铈的混合物上来合成几种新型材料,以研究在FeO x / ZrO 2材料中添加CeO 2在热化学水分解反应中的作用。在1000℃(在1450℃下热还原后)的水分解的温度下,铈的稳定性2含材料比为FeO的下X /的ZrO 2材料,并没有优势的CeO加入2到FeO x / ZrO 2材料。但是,当在1200°C的水分解(WS)温度下操作时,与1000°C的水分解温度相比,大多数材料的稳定性提高,并且氢气产生量显着更高。在WS温度为1200°C时,FeO x / Zr 75 Ce 25 O 2(按重量计75%Zr 75 O 2和25%CeO 2)和FeO x / Zr 50 Ce 50 O 2材料的性能略好于FeO。x / ZrO 2材料和X射线光电子能谱数据显示,与在1000°C下进行水分解相比,铁的表面协调作用不那么重要。程序升温还原数据表明,FeO x -CeO 2的相互作用比FeO x -ZrO 2的相互作用弱,因为FeO x的还原发生在含CeO 2的材料较低的温度下。较弱的相互作用可以解释为什么含CeO 2的材料的稳定性较低(FeO x的烧结可能更明显)。X射线衍射数据表明ZrO 2 -CeO 2在1450°C活化后形成的固溶体和晶格体积计算表明,铁确实掺入了ZrO 2 -CeO 2基质中。与较低的温度(1000°C)相比,在1200°C的水分解后观察到更多的掺入,这可能解释了为什么在1200°C的水分解过程中材料更稳定。

更新日期:2018-06-19
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