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高水热稳定有序介孔Al-SBA-15材料的优化合成及表征
  • ISSN号:0251-0790
  • 期刊名称:高等学校化学学报
  • 时间:2015
  • 页码:2355-2363
  • 分类:O613[理学—无机化学;理学—化学] O643[理学—物理化学;理学—化学]
  • 作者机构:太原理工大学化学化工学院,能源化工与催化研究中心,太原030024
  • 相关基金:国家自然科学基金(批准号:51172154,51451002)和山西省青年基础研究基金(批准号:2012021006-2,2013021008-3)资助.
  • 相关项目:多级中微孔锆铝氧化物(分子筛)的合成及其性能研究
作者: 李瑞丰|
中文摘要:

借助无机铝盐自水解所产生的弱酸性环境,通过改变水热处理温度及无机铝盐的引入种类和引入量来调控合成体系中Al—OH及材料孔壁中Si—OH的相对含量,在不引入矿物质强酸的条件下,一步合成了具有高Al引入量且孔壁硅、铝物种达到原子水平均匀分散的Al-SBA-15介孔材料.表征结果表明,当以硝酸铝为铝源,水热处理温度和投料硅铝比分别为140℃和10时,所得样品具有高度有序的二维六方介孔结构及较高的水热稳定性,在经800℃高温水蒸气处理2 h后,其介孔比表面积和孔体积仅分别降低了18.82%和16.67%.此外,骨架Al的引入使所得样品同时具有B酸和L酸中心,且具有相对较强的酸性,在异丙苯催化裂化反应中表现出明显活性.

英文摘要:

Highly ordered mesoporous Al-SBA-15 materials with high aluminum content and high hydrother- mal stability were synthesized by one-step hydrothermal grafting approach under the weak acid medium produced only by the hydrolysis of inorganic aluminum salt. By selectively introducing inorganic aluminum salt in the synthesis system, and further optimizing hydrothermal treatment temperature and the introduced amount of inorganic aluminum salt, the hydrolysis of Al ion and the condensation of silicon hydroxyl(Si-OH) species within the mesoporous wails could be efficiently controlled to adjust the relative amount of Al-OH and Si-OH groups and their interaction. As a result, the ordered mesostructure of Al-SBA-15 could be assem- bled at the mesoscale and the coordination status/the acidic sites could be controlled at the atomic scale. The characteristic results by means of XRD, N2 adsorption, TEM, EDX, SEM, FTIR and NMR techniques showed that when aluminium nitrate was used as the aluminum precursor, and hydrothermal treatment temperature and initial molar ratio of silicate to aluminium were adjusted as 140 ℃ and 10, respectively, the synthesized sample exhibited highly ordered hexagonal mesostructure and extremely high hydrothermal stability. The highly ordered mesostructure can be maintained even after steam treatment at 800 % for 2 h with only 18.82% and 16.67% decreases in the Brunauer-Emmett-Teller surface area and total pore volume, respectively. Moreover, the hydrothermal grafting process at 140 ℃ was advantageous for the homogeneous incorporation of Al into the silica mesoporous framework to form the Si-OH-Al bond, leading to the production of Brensted and Lewis acid sites with relatively strong acidity on the mesoporous walls.

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期刊信息
  • 《高等学校化学学报》
  • 北大核心期刊(2011版)
  • 主管单位:中华人民共和国教育部
  • 主办单位:吉林大学 南开大学
  • 主编:周其凤
  • 地址:吉林大学南胡校区
  • 邮编:130012
  • 邮箱:cjcu@jlu.edu.cn
  • 电话:0431-88499216
  • 国际标准刊号:ISSN:0251-0790
  • 国内统一刊号:ISSN:22-1131/O6
  • 邮发代号:12-40
  • 获奖情况:
  • 首届及第二届国家期刊奖,连续两届“百种中国杰出学术期刊”,中国期刊方阵“双高”期刊
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:50676