制备方法对Ni/Al<sub>2</sub>O<sub>3</sub>-SiC泡沫结构催化剂Ni分布和苯甲醛加氢性能的影响

doi:10.11901/1005.3093.2018.317

材料研究学报

2018, Vol. 32

Issue (11): 811-819 DOI: 10.11901/1005.3093.2018.317

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制备方法对Ni/Al₂O₃-SiC泡沫结构催化剂Ni分布和苯甲醛加氢性能的影响

李恺^1,², 矫义来¹, 杨振明¹, 张劲松¹(

)

1 沈阳材料科学国家研究中心中国科学院金属研究所沈阳 110016
2 中国科学院大学北京 100049

Effect of Preparation Methods on Ni-distribution and Catalytic Performance of Foam Structured Catalyst Ni/Al₂O₃-SiC for Hydrogenation of Benzaldehyde

Kai LI^1,², Yilai JIAO¹, Zhenming YANG¹, Jinsong ZHANG¹(

)

1 Shenyang National Research Center for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2 University of Chinese Academy of Sciences, Beijing 100049, China

引用本文:

李恺, 矫义来, 杨振明, 张劲松. 制备方法对Ni/Al₂O₃-SiC泡沫结构催化剂Ni分布和苯甲醛加氢性能的影响[J]. 材料研究学报, 2018, 32(11): 811-819.
Kai LI, Yilai JIAO, Zhenming YANG, Jinsong ZHANG. Effect of Preparation Methods on Ni-distribution and Catalytic Performance of Foam Structured Catalyst Ni/Al₂O₃-SiC for Hydrogenation of Benzaldehyde[J]. Chinese Journal of Materials Research, 2018, 32(11): 811-819.

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摘要:

采用浸渍法和沉积-沉淀法制备了Ni为催化活性组分的Ni/Al₂O₃-SiC泡沫结构催化剂,使用扫描电镜能谱(SEM-EDS)、X射线衍射(XRD)、N₂吸附-脱附、透射电镜(TEM)、X射线光电子能谱(XPS)和程序升温还原(H₂-TPR)等手段表征结构催化剂,研究了活性组分制备方法对Ni分布、Ni颗粒尺寸、元素价态以及Ni与载体之间相互作用的影响,并考察了用不同方法制备的结构催化剂的苯甲醛液相加氢性能。结果表明,在40℃、160℃和真空冻干三种不同条件下干燥的浸渍型结构催化剂,在其涂层表面出现了不同程度的Ni富集,在160℃干燥的催化剂涂层表面Ni的富集最严重。与浸渍法相比,用沉积-沉淀法制备的结构催化剂其活性组分Ni的分布更均匀,Ni颗粒的尺寸更小,具有更高的苯甲醛加氢性能。

关键词 ：无机非金属材料, 催化材料, 结构催化剂, Al₂O₃涂层, Ni分布, 苯甲醛加氢

Abstract：

The foam structured catalysts of Ni/Al₂O₃-SiC were prepared via conventional impregnation (IM) and deposition-precipitation (DP) methods. These catalysts were characterized by means of scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), X-ray diffraction (XRD), N₂ absorption-desorption, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and H₂temperature-programmed reduction (H₂-TPR). The effect of preparation methods on the distribution, particle size and valence state of the active component Ni, as well as the interaction between Ni and the supporter was investigated. Furthermore, the catalytic performance of the catalysts prepared by different methods was evaluated for the liquid-phase hydrogenation of benzaldehyde. Results show that the Ni enrichment occurred on the coating surface of three catalysts prepared via impregnating and then dried in air at 40℃ and 160℃, as well as subjected to vacuum freeze-drying, respectively. The foam catalyst dried at 160℃ showed the most serious enrichment of Ni on the coating surface. Compared with the three impregnated foam catalysts, the catalyst prepared by DP method has a uniform Ni distribution and smaller Ni particles size, leading to its higher catalytic performance for hydrogenation of benzaldehyde.

Key words： inorganic non-metallic materials catalytic materials structured catalysts Al₂O₃ coating Ni distribution benzaldehyde hydrogenation

收稿日期: 2018-05-11

ZTFLH:

TQ426

基金资助:国家重点研发计划重点专项(2017YFB0310405)

作者简介:

作者简介李恺,男,1985年生,博士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2018.317 或 https://www.cjmr.org/CN/Y2018/V32/I11/811

图1 苯甲醛的选择加氢反应路径

图2 SiC泡沫陶瓷和Al2O3-SiC泡沫结构载体的SEM照片

图3 不同方法制备的Ni/A25S结构催化剂涂层横截面的SEM照片和涂层径向上的Ni分布

图4 不同方法制备的Ni/A25S结构催化剂涂层外表面的SEM照片和涂层外表面的Ni分布

图5 不同方法制备的结构催化剂的XRD图谱

表1 结构催化剂的物性参数

图6 不同方法制备的结构催化剂的TEM照片

图7 不同方法制备的结构催化剂中Ni 2p的XPS精细谱图

图8 不同方法制备的未活化催化剂的H2-TPR图谱

图9 不同方法制备的Ni/A25S结构催化剂的苯甲醛加氢性能

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