杂多阴离子柱撑类水滑石的合成、表征及催化研究

郑建华; 庞海霞; 王长杰; 姜燕冬; 赵军丽; 贾云龙

杂多阴离子柱撑类水滑石的合成、表征及催化研究

中国地质大学材料科学与化学工程学院, 湖北武汉 430074

详细信息

作者简介:
郑建华(1954-), 女, 副教授, 主要从事有机化学的研究.E-mail: phx2001253@163.com

中图分类号: P619.2
计量
- 文章访问数: 3309
- HTML全文浏览量: 91
- PDF下载量: 2
- 被引次数: 0
出版历程
- 收稿日期: 2003-09-23
- 刊出日期: 2004-03-25

Study on Synthesis, Characterization and Catalysis of Heteropolyanion Pillared Hydrotalcite-Like Compounds

Faculty of Material Science and Chemical Engineering, China University of Geosciences, Wuhan 430074, China

摘要

摘要: 采用共沉淀法合成了具有不同组成的类水滑石层状化合物和杂多酸, 并以此制备了一系列杂多阴离子柱撑类水滑石; 用XRD和IR方法对柱撑产物的结构进行了表征, 它们具有K结构; 结果表明这些材料层间高度为0.97nm.并且发现以H₂O₂为氧化剂的这种层柱催化剂在液-固相中对苯甲醛氧化成苯甲酸具有很高的活性和选择性.
- 杂多阴离子 /
- 类水滑石 /
- 制备 /
- 苯甲醛 /
- H₂O₂氧化
Abstract: Hydrotalcite-like compounds, heteropolyanions with different compositions, and their pillared products were synthesized by coprecipitation. The structures were characterized by XRD and IR with Keggin structure. The results indicated that these materials possess exceptionally well-ordered gallery height of 0.97 nm. It is found that this kind of pillared layered catalyst has high activity and selectivity for the oxidation of benzaldehyde to benzoic acid using H₂O₂ as oxidant in liquid-solid phase system.
- heteropolyanion /
- hydrotalcite-like compound /
- preparation /
- benzaldehyde /
- H₂O₂ oxidation

HTML全文

图 1 Zn₂Al-TA的XRD谱图

Fig. 1. XRD patterns of Zn₂Al-TA

下载: 全尺寸图片幻灯片

图 2 PZW₁₁的IR谱图

(1)PCoW₁₁;(2)PNiW₁₁;(3)PCuW₁₁

Fig. 2. IR spectra of PZW₁₁

下载: 全尺寸图片幻灯片

图 3 Zn₂Al-PZW₁₁的XRD谱图

Fig. 3. X-ray diffraction patterns of Zn₂Al-PZW₁₁

下载: 全尺寸图片幻灯片

图 4 Zn₂Al-PZW₁₁的IR谱图

Fig. 4. IR spectra of Zn₂Al-PZW₁₁

下载: 全尺寸图片幻灯片

表 1 Zn₂Al-A^n-的d(003)实验值与预想值比较

Table 1. Comparison of expected with observed d(003)spacings of Zn₂Al-A^n- having various anions

表 2 Zn₂Al-PZW₁₁的IR光谱数据

Table 2. IR data of Zn₂Al-PZW₁₁ cm^-1

表 3 Zn₂Al-PZW₁₁对苯甲醛的H₂O₂氧化催化活性

Table 3. Catalytic activity of Zn₂Al-PZW₁₁ for oxidation of benzaldehyde to benzoic acid using H₂O₂ as oxidant

参考文献(16)

[1]	Cavani, F., Trifiro, F., Vaccari, A., 1991. Hydrotalcite-type anionic clays: Preparation, properties and application. Catal Today, 11: 173-301. doi: 10.1016/0920-5861(91)80068-K
[2]	Drezdzon, M. A., 1988. Synthesis of isopolymetalate-pillared hydrotalcite via organic-anion-pillared precursors. Inorg. Chem., 27: 4628-4632. doi: 10.1021/ic00298a024
[3]	He, Q. L., Hu, C. W., Zhang, Y. F., et al., 1996a. Studies on the oxidative activity and thermal stability of a new type pillared layered catalyst Zn₂Al-XW₁₁Z. Chinese Journal of Catalysis, 17(6): 559-562(in Chinese with English abstract).
[4]	He, Q. L., Hu, C. W., Zhang, Y. F., et al., 1996b. Study on the synthesis, characterization and catalysis of pillared anion clay(Ⅴ). Acta Physico-Chimica Sinica, 12(4): 368-371(in Chinese with English abstract). doi: 10.3866/PKU.WHXB19960417
[5]	Hu, C. W., He, Q. L., Xie, G. X., et al., 1996a. Studies on the oxidative activity of a new type pillared layered catalyst Zn₂Al-GeW₁₁Z for the oxidation of liquid-solid phase of benzaldehyde using H₂O₂. Journal of Northeast Normal University(Natural Science Edition), 1: 122(in Chinese with English abstract).
[6]	Hu, C. W., He, Q. L., Zhang, Y. F, et al., 1996b. New route for preparation of layer-pillared catalyst [Zn₂Al(OH)₂]·[SiW₁₁O₃₉Co(H₂O)]_0.83·4H₂O and its catalytic activities for the oxidation of benzaldehyde using H₂O₂ as oxidant. Journal of Molecular Catalysis, 10(1): 67-69(in Chinese with English abstract).
[7]	Hu, C. W., Liu, Y. Y., Wang, Z. P., et al., 1995. New type micropore material—Study on synthesis, characterization, oxidative activety and catalysis of Zn-Al heteropolyanion pillared anion clay. Science in China(Series B), 25: 916-922(in Chinese with English abstract).
[8]	Liu, P., Zheng, J. H., Pi, Z. B., et al., 2003. Synthesis and characterization of magnesium-aluminum-indium hydrotalcite-like compounds. Earth Science—Journal of China University of Geosciences, 28(2): 163-166(in Chinese with English abstract).
[9]	Narita, E., Kaviratna, P. D., Pinnavaia, T. J., 1993. Direct synthesis of a polyoxometallate-pillared layered double hydroxide by coprecipitation. J. Chem. Soc., Chem. Commun., 1: 60-62.
[10]	Weakley, T. J. R., Malik, S. A., 1967. Heteropolyanions containing two different heteroatoms-Ⅰ. J. Inorg. Nucl. Chem., 29: 2935-2944. doi: 10.1016/0022-1902(67)80126-X
[11]	贺庆林, 胡长文, 张云峰, 等, 1996a. 新型层柱催化剂Zn₂Al-XW₁₁Z的催化氧化活性及热稳定性. 催化学报, 17(6): 559-562. https://www.cnki.com.cn/Article/CJFDTOTAL-CHUA606.022.htm
[12]	贺庆林, 胡长文, 张云峰, 等, 1996b. 柱撑阴离子粘土的合成、表征及催化性能研究(Ⅴ). 物理化学学报, 12(4): 368-371. https://www.cnki.com.cn/Article/CJFDTOTAL-WLHX199503000.htm
[13]	胡长文, 贺庆林, 谢告雪, 等, 1996a. 新型层柱催化剂Zn₂Al-GeW₁₁Z对苯甲醛的H₂O₂液-固相氧化活性. 东北师大学学报自然科学版(研究简报), 1: 122. https://www.cnki.com.cn/Article/CJFDTOTAL-DBSZ601.029.htm
[14]	胡长文, 贺庆林, 张云峰, 等, 1996b. 层柱催化剂[Zn₂Al·(OH)₂][SiW₁₁O₃₉Co(H₂O)]_0.83·4H₂O的合成新途径及其对苯甲醛H₂O₂氧化的催化活性. 分子催化, 10(1): 67-69.
[15]	胡长文, 刘彦勇, 王作屏, 等, 1995. 新型微孔材料——杂多阴离子柱撑Zn-Al型阴离子粘土的合成、表征及其催化反应活性研究. 中国科学(B辑), 25: 916-922. https://www.cnki.com.cn/Article/CJFDTOTAL-JBXK199509003.htm
[16]	刘鹏, 郑建华, 皮振邦, 等, 2003. 镁铝铟类水滑石的合成与表征. 地球科学——中国地质大学学报, 28(2): 163-166. https://www.cnki.com.cn/Article/CJFDTOTAL-DQKX200302008.htm