催化学报 ›› 2014, Vol. 35 ›› Issue (12): 1927-1936.DOI: 10.1016/S1872-2067(14)60129-7

• 论文 • 上一篇    下一篇

不同有机分子改性羟基磷灰石用于甲醛催化氧化

孙亚会a, 曲振平a, 陈丹a, 王辉a, 张帆b, 傅强b   

  1. a. 大连理工大学环境学院工业生态与环境工程教育部重点实验室, 辽宁大连116024;
    b. 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连116023
  • 收稿日期:2014-04-13 修回日期:2014-04-28 出版日期:2014-11-29 发布日期:2014-11-29
  • 通讯作者: 曲振平
  • 基金资助:

    国家自然科学基金(21377016); 中央高校基本科研业务费专项资金(DUT13LK27); 长江学者和创新团队发展计划 (IRT_13R05).

Formaldehyde catalytic oxidation over hydroxyapatite modified with various organic molecules

Yahui Suna, Zhenping Qua, Dan Chena, Hui Wanga, Fan Zhangb, Qiang Fub   

  1. a. Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian116024, Liaoning, China;
    b. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • Received:2014-04-13 Revised:2014-04-28 Online:2014-11-29 Published:2014-11-29
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21377016), the Fundamental Research Funds for the Central Universities (DUT13LK27), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT_13R05).

摘要:

分别采用十六烷基三甲基溴化铵(CTAB)、十二烷基硫酸钠(SDS)及柠檬酸钠(SC)对羟基磷灰石(HAP)进行了有机改性.柠檬酸钠改性的羟基磷灰石对甲醛催化氧化表现出最好的催化活性, 在240 ℃实现了甲醛完全转化.通过X射线衍射、红外光谱、N2吸附-脱附、扫描电镜和热重/差重等手段对HAP结构进行了表征.结果表明, SC改性使得HAP比表面积和孔体积增加, 孔径减小, 更有利于吸附及传质, 从而提高了其活性.此外, SC改性的HAP中羟基含量更多, 更有利于甲醛与羟基之间发生相互作用, 这是该样品活性提高的另一个原因.

关键词: 羟基磷灰石改性, 柠檬酸钠, 比表面积, 羟基, 甲醛催化氧化

Abstract:

Hydroxyapatite (HAP) was modified by adding various organic molecules, such as cetyltrimethylammonium bromide, sodium dodecyl sulfate, and sodium citrate, during the precipitation of HAP. Sodium citrate-modified HAP displayed the best activity for formaldehyde oxidation, achieving complete conversion at 240 ℃. The influence of the organic modifiers on the structure of HAP was assessed by X-ray diffraction, Fourier transform infrared spectroscopy, N2 adsorption- desorption, scanning electron microscopy, and thermogravimetry/derivative thermogravimetry. The higher specific surface area and pore volume, and smaller pores, owing to modification with sodium citrate, favored adsorption, mass transfer, and interaction process during formaldehyde oxidation. Furthermore, the higher hydroxyl group content observed in sodium citrate- modified HAP enhanced interactions between formaldehyde and HAP, thus resulting in higher catalytic activity.

Key words: Modified hydroxyapatite, Sodium citrate, Specific surface area, Hydroxyl group, Formaldehyde catalytic oxidation