K改性Ni-Co-Al三元复合氧化物催化分解N<sub>2</sub>O

武海鹏; 冯鸣; 徐秀峰

K改性Ni-Co-Al三元复合氧化物催化分解N₂O

烟台大学应用催化研究所, 山东烟台 264005

基金项目: 教育部留学回国人员科研启动基金(2004-527); 煤转化国家重点实验室开放基金(06-603)。

详细信息

通讯作者:
徐秀峰,Tel: 0535-6902746, E-mail: xxf@ytu.edu.cn.

中图分类号: O643
计量
- 文章访问数: 2539
- HTML全文浏览量: 27
- PDF下载量: 838
- 被引次数: 0
出版历程
- 收稿日期: 2011-10-17
- 修回日期: 2011-12-29
- 刊出日期: 2012-07-31

Catalytic decomposition of N₂O over potassium promoted Ni-Co-Al ternary mixed oxides

Institute of Applied Catalysis, Yantai University, Yantai 264005, China

摘要

摘要: 制备了(Ni+Co)/Al=3、Ni/Co=0.2(原子比)的NiCoAl三元类水滑石样品,焙烧获得NiCoAl复合氧化物,表面浸渍K₂CO₃溶液制备了K改性催化剂,用于N₂O分解反应,考察了K负载量、焙烧温度等制备参数和O₂、H₂O等反应气氛对催化剂活性的影响。用BET、XRD、H₂-TPR、XPS等技术表征了催化剂的组成结构。结果表明,K的表面改性提高了催化剂对N₂O分解反应的催化活性,其中,400℃预焙烧NiCoAl类水滑石制得复合氧化物,初湿浸渍K₂CO₃溶液,K的负载量为K/(Ni+Co)=0.05,400℃ 再焙烧制备的催化剂活性较高,有氧有水条件下500℃ 反应时N₂O可完全分解;在NiCoAl复合氧化物表面负载K₂CO₃组分,降低了催化剂表面Co、Ni元素的电子结合能,弱化了表面Co-O、Ni-O化学键,从而提高了催化剂活性和抗水性能。
- N₂O催化分解 /
- K改性NiCoAl复合氧化物 /
- 催化剂制备参数 /
- 反应气氛 /
- 催化活性
Abstract: NiCoAl ternary mixed oxides derived from hydrotalcite-like compounds (HLc) with (Ni+Co)/Al atomic ratio of 3 and Ni/Co of 0.2 were incipiently impregnated by potassium carbonate solution to prepare K-promoted NiCoAl mixed oxides for catalytic decomposition of N₂O. The effects of catalyst preparation parameters such as K loadings, calcination temperatures, and reaction atmospheres on catalytic activity were investigated. The catalysts were characterized by BET, XRD, H₂-TPR, and XPS techniques. The results show that the catalytic activity of NiCoAl mixed oxides is largely enhanced by the addition of K species in the presence of oxygen and steam, and the optimal catalyst preparation parameters are K/(Ni+Co) atomic ratio of 0.05 and calcination temperature of 400℃. XPS and H₂-TPR data show that the electron binding energy of active Co₃O₄ and NiO species over K-promoted catalysts surface shifted to lower value, indicating the surface Co-O and Ni-O bonds were weakened, thus the reduction peaks of Co³⁺ to Co²⁺ and Ni²⁺ to Ni⁰ moved to lower temperature, and the catalytic activity and resistance towards water is improved.
- N₂O catalytic decomposition /
- K-promoted NiCoAl mixed oxides /
- catalyst preparation parameters /
- reaction atmosphere /
- catalytic activity

HTML全文

参考文献(16)

OBALOVA L, FILA V. Kinetic analysis of N₂O decomposition over calcined hydrotalcites[J]. Appl Catal B, 2007, 70(1/4): 353-359.

ASANO K, OHNISHI C, IWAMOTO S, SHIOYA Y, INOUE M. Potassium-doped Co₃O₄ catalyst for direct decomposition of N₂O[J]. Appl Catal B, 2008, 78(3/4): 242-249.

OHNISHI C, ASANO K, IWAMOTO S, CHIKAMA K, INOUE M. Alkali-doped Co₃O₄ catalysts for direct decomposition of N₂O in the presence of oxygen[J]. Catal Today, 2007, 120(2): 145-150.

STELMACHOWSKI P, MANIAK G, KOTARBA A, SOJKA Z. Strong electronic promotion of Co₃O₄ towards N₂O decomposition by surface alkali dopants[J]. Catal Commun, 2009, 10(7): 1062-1065.

PASHA N, LINGAIAH N, REDDY P S S, PRASAD P S S. Direct decomposition of N₂O over cesium-doped CuO catalysts[J]. Catal Lett, 2009, 127(1/2): 101-106.

PASHA N, LINGAIAH N, BABU N S, REDDY P S S, PRASAD P S S. Studies on cesium doped cobalt oxide catalysts for direct N₂O decomposition in the presence of oxygen and steam[J]. Catal Commun, 2008, 10(2): 132-136.

PASHA N, LINGAIAH N, REDDY P S S, PRASAD P S S. An investigation into the effect of Cs promotion on the catalytic activity of NiO in the direct decomposition of N₂O[J]. Catal Lett, 2007, 118(1/2): 64-68.

YAN L, REN T, WANG X, JI D, SUO J. Catalytic decomposition of N₂O over M_xCo_1?xCo₂O₄ (M = Ni, Mg) spinel oxides[J]. Appl Catal B, 2003, 45(2): 85-90.

CHANG K S, SONG H, PARK Y S, WOO J W. Analysis of N₂O decomposition over fixed bed mixed metal oxide catalysts made from hydrotalcite-type precursors[J]. Appl Catal A, 2004, 273(1/2): 223-231.

OBALOVA L, KARASKOVA K, JIRATOVA K, KOVANDA F. Effect of potassium in calcined Co-Mn-Al layered double hydroxide on the catalytic decomposition of N₂O[J]. Appl Catal B, 2009, 90(1/2): 132-140.

KARASKOVA K, OBALOVA L, JIRATOVA K, KOVANDA F. Effect of promoters in Co-Mn-Al mixed oxide catalyst on N₂O decomposition[J]. Chem Eng J, 2010, 160(2): 480-487.

KOVANDA F, ROJKA T, BEZDIOKA P, JIRÁTOVA K, OBALOVá L, PACULTOVá K, BASTL Z, GRYGAR T. Effect of hydrothermal treatment on properties of Ni-Al layered double hydroxides and related mixed oxides[J]. J Solid State Chem, 2009, 182(1): 27-36.

CHENG H, HUANG Y, WANG A, LI L, WANG X, ZHANG T. N₂O decomposition over K-promoted Co-Al catalysts prepared from hydrotalcite-like precursors[J]. Appl Catal B, 2009, 89(3/4): 391-397.

武海鹏, 钱振英, 徐晓玲, 徐秀峰. K改性NiAl类水滑石衍生复合氧化物催化分解N₂O[J]. 燃料化学学报, 2011, 39(2): 115-121. (WU Hai-peng, QIAN Zhen-ying, XU Xiao-ling, XU Xiu-feng. N₂O decomposition over K-promoted NiAl mixed oxides derived from hydrotalcite-like compounds[J]. Journal of Fuel Chemistry and Technology, 2011, 39(2): 115-121.)

徐晓玲, 徐秀峰, 张国涛, 牛宪军. 钴铝复合氧化物负载金催化剂的制备及催化分解N₂O[J]. 燃料化学学报, 2009, 37(5): 595-600. (XU Xiao-ling, XU Xiu-feng, ZHANG Guo-tao, NIU Xian-jun. Preparation of Co-Al mixed oxide supported gold catalysts and their catalytic activity for N₂O decomposition[J]. Journal of Fuel Chemistry and Technology, 2009, 37(5): 595-600.)

YAN L, REN T, WANG X, GAO Q, JI D, SUO J. Excellent catalytic of Zn_xCo_1-xCo₂O₄ spinel catalyst for the decomposition of nitrous oxide[J]. Catal Commun, 2003, 4(10): 505-509.

施引文献

资源附件(0)

访问统计