化学学报 ›› 2012, Vol. 70 ›› Issue (18): 1957-1962.DOI: 10.6023/A12060321 上一篇    下一篇

研究论文

氨基表面功能化的有序介孔杂合材料的一步法合成及其对重金属离子和CO2 的吸附特性

邵悦, 马勇   

  1. 渤海大学化学化工与食品安全学院 锦州 121013
  • 投稿日期:2012-06-18 发布日期:2012-08-29
  • 通讯作者: 马勇
  • 基金资助:

    项目受渤海大学辽宁省高校重大科技平台“食品贮藏加工及质量安全控制工程技术研究中心”、“辽宁省食品安全重点实验室”开放课题(No.LNSAKF2011027)和辽宁省教育厅重点实验室(No. 2009s004)资助.

Amino Group Surface-functionalized Ordered Mesoporous Materials:One-pot Synthesis, Heavy-metal Ion and CO2 Adsorption

Shao Yue, Ma Yong   

  1. College of Chemistry, Chemical Engineering and Food Safety, Bohai University, Jinzhou 121013
  • Received:2012-06-18 Published:2012-08-29
  • Supported by:

    Supporting information for this article is available free of charge via the Internet at http://sioc-journal.cn. Project supported by the Engineering and Technology Research Center of Food Preservation, Processing and Safety Control of Liaoning Province, Food Safety Key Lab of Liaoning Province (LNSAKF2011027), and Key Laboratory Project of Department of Education of Liaoning Province (2009s004).

以F127 为表面活性剂, 通过(4-氨基-1-羟基亚丁基)二膦酸单钠盐三水合物与TiCl4 一步法缩合反应制得有序介孔杂合材料. 通过TEM 图像可观察到所制备的材料具有六方有序介孔结构, 氮气吸附分析测得其比表面积高达420m2·g-1, 孔径分布均匀, 最可几孔径为6.9 nm. FT-IR 和MAS NMR 表明有机官能团进入介孔材料骨架中. 由于所合成的材料表面含有丰富的氨基官能团, 可以与诸如Hg2+, Pb2+和Cd2+等重金属离子发生络合作用, 所以这种杂合材料可以作为一种优秀的离子吸附剂, 其吸附行为可归属于Langmuir 吸附类型. 同时, 由于该材料中含氨基和羟基官能团,对CO2 的捕获有较大贡献, 测试得知CO2 吸附量可达2.47 mmol·g-1, 并具有高稳定性和选择性.

关键词: 介孔材料, 功能化, 重金属, CO2, 选择性

Mesoporous materials have attracted more and more attention and shown great potentials in many fields, due to their outstanding properties including high surface areas, periodically arranged mesopore space, tunable pore sizes, alternative pore shapes and uniform nanosized frameworks. In this article, a simple one-pot hydrothermal strategy was applied to prepare periodic mesoporous amino group functionalized materials in the presence of nonionic block copolymer surfactant F127. Ordered hexagonal mesopores were observed from the TEM observations, with the high surface area and the uniform pore size distribution. FT-IR and MAS NMR could confirm that the functional groups were incorporated into the network of the mesoporous solids. Different experimental parameters including the adding amount of surfactant F127, the molar ratio of precursors, and the acidity of the reaction solution were investigated. And we found that the highly ordered hexagonal mesoporous materials could be prepared at pH≈3, F127 adding amount of 1.5~2.5 g and 0.2 < P/Ti < 0.4. Heavy metal ions are proved to be highly toxic environmental pollutants, harmful to the health of human beings even at very low concentrations in the water. Thus the synthesized materials were used as efficient adsorbents for heavy metal ions such as Hg2+, Pb2+ and Cd2+ions, which followed Langmuir-type behavior. The synthesized adsorbents also had some selectivity for Hg2+and Pb2+over Cd2+ions. The adsorption capacity exhibited no obvious decrease after six multiple use cycles, showing well stability. With the increasing of carbon dioxide, undesirable consequence for the Earth’s environment is caused by the alteration of the temperature of the atmosphere and the acidity of the oceans. The capture of CO2 and its storage may play a very important role for decreasing its emissions to the atmosphere. Therefore, the synthesized materials were also proved to be useful in CO2 capture benefiting from abundant amino and hydroxyl groups, showing the large adsorption capacity with high stability and selectivity. The present method is expected to open a new pathway to prepare amino group functionalized mesoporous adsorbents other than silica-based materials.

Key words: mesoporous materials, functionalization, heavy metal, CO2, selectivity