Zn 掺杂的 LaCoO3 钙钛矿用于乙醇水蒸气重整制氢反应

doi:10.1016/S1872-2067(10)60218-5

摘要/Abstract

摘要： 利用一步柠檬酸络合法合成了钙钛矿 LaCo_1-xZn_xO₃ (x = 0, 0.05, 0.1, 0.2, 0.3 and 0.5), 并将其用于乙醇水蒸气重整反应. 利用 X 射线衍射、程序升温还原和 X 射线光电子能谱对催化剂进行了表征. 结果表明, Zn 的加入不利于形成 LaCo_1-xZn_xO₃ 钙钛矿结构, 当 x ≥ 0.1 时产生了一些分离相. 新鲜 LaCo0.9Zn0.1O3 催化剂中意外发现存在 Co₃O₄ 相, 这有利于催化剂反应性能的提高. 反应后的催化剂结构发生变化, 形成了 La₂O₂CO₃, 而该物质有利于积炭的消除和甲烷的重整.

关键词: 一步柠檬酸络合法, 钙钛矿, 多样纳米核, 锌, 乙醇, 蒸气重整, 积炭

Abstract: Nanostructured LaCo_1-xZn_xO₃ (x = 0, 0.05, 0.1, 0.2, 0.3 and 0.5) perovskites were synthesized by a one-step citric acid-complexing method for hydrogen production by the steam reforming of ethanol. For comparison, 8% CoO/ZnO and 8% CoO/La₂O₃ were prepared by impregnation and evaluated. The catalyst samples were characterized by X-ray diffraction, temperature-programmed reduction, and X-ray photoelectron spectroscopy. The results indicated that zinc did not favor the formation of the LaCo_1-xZn_xO₃ perovskite and the structures of the substituted samples were stronger than that of LaCoO₃. Some segregation was observed for x ≥ 0.1. The reactivity of the studied samples was sensitive to the zinc content and lower substitution values were found to be better. An unexpected phase (Co₃O₄) appeared in the fresh LaCo_0.9Zn_0.1O₃ sample. The presence of the Co₃O₄ phase increased the reactivity toward hydrogen production by the steam reforming of ethanol. The presence of La₂O₂CO₃ is responsible for the low carbon deposition and the CH₄ selectivity in the aged samples.

Key words: one-step citric acid-complexing method, perovskite, multiple nanosized-cores, zinc, ethanol, steam reforming, carbon deposition

马飞, 储伟, 黄利宏, 余晓鹏, 吴永永. Zn 掺杂的 LaCoO3钙钛矿用于乙醇水蒸气重整制氢反应[J]. 催化学报, 2011, 32(6): 970-977.

MA Fei, CHU Wei, HUANG Li-Hong, YU Xiao-Peng, WU Yong-Yong. Steam Reforming of Ethanol over Zn-Doped LaCoO₃ Perovskite Nanocatalysts[J]. Chinese Journal of Catalysis, 2011, 32(6): 970-977.

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