高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

晶种辅助蒸汽转化Al-SBA-15合成Beta纳米晶团聚体

孙琳1,林森1,王润伟2   

  1. 1. 青岛科技大学，材料科学与工程学院，青岛 266042；
    2. 无机合成与制备化学国家重点实验室，吉林大学化学学院，长春 130012
  • 收稿日期:2024-03-06 修回日期:2024-04-19 网络首发:2024-04-22 发布日期:2024-04-22
  • 通讯作者: 林森 E-mail:03071@qust.edu.cn
  • 基金资助:
    山东省自然科学基金(批准号: ZR2022MB030)和国家自然科学基金(批准号: 21390394, 21771082, 21771081, 21703128, 51472256)资助.

Synthesis of Beta nanocrystal aggregates from Al-SBA-15 via seed-assisted steaming conversion

SUN Lin1, LIN Sen1, WANG Runwei2   

  1. 1. College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China; 2. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
  • Received:2024-03-06 Revised:2024-04-19 Online First:2024-04-22 Published:2024-04-22
  • Contact: LIN Sen E-mail:03071@qust.edu.cn
  • Supported by:
    Supported by the Shandong Provincial Natural Science Foundation, China(No. ZR2022MB030) and the National Natural Science Foundation of China(Nos. 21390394, 21771082, 21771081, 21703128, 51472256).

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摘要： 本研究将有序介孔分子筛Al-SBA-15颗粒直接转化为Beta纳米晶团聚体（Beta Nanocrystal Aggregates，BNA），合成方法：Seed-Assisted Steaming Conversion策略，简称SASC。除规则微孔外，Beta纳米晶团聚体含有两种多级介孔结构。采用多样表征技术系统研究了合成过程中骨架组装与多级孔结构的演化过程。调节热分解条件，将P123胶束选择性碳化生成碳颗粒高分散于有序介孔内，在Al-SBA-15颗粒中构建新的三维纳米空间网格。使用蒸汽处理方法将Al-SBA-15无定形孔壁在这些纳米空间中缓慢转化为Beta纳米晶体。调节热力学参数，控制纳米晶沿Al-SBA-15孔壁方向排列，生成有序介观结构。此外，高温焙烧去除碳颗粒后，BNA内部生成穴状介孔。使用低溶剂含量的反应介质能够大大降低传质速度，显著提高骨架组装质量，Beta纳米晶团聚体显示出优异酸性质。

关键词: 多级孔Beta, Al-SBA-15, 晶种辅助蒸汽转化, 骨架组装

Abstract: Beta nanocrystal aggregates (BNA) possessing two types of hierarchical mesopores have been successfully synthesized by one-step conversion of the ordered mesoporous material Al-SBA-15 following a seed-assisted steaming conversion (SASC) strategy. The relationship between the assembly of the Beta zeolite and the evolution of hierarchical mesostructure was investigated. Using a controllable thermal treatment, the P123 micelle was selectively decomposed to form the carbonaceous particles that highly dispersed inside the mesopores, and then constructed a new three-dimensional nanosized space network in the whole Al-SBA-15 bulky particles. With the help of the pre-impregnated Beta seed solution and TEA+ template, the amorphous Al-SBA-15 walls were slowly converted to the Beta nanocrystals in these spaces under the low-solvent-content conditions. The resulting nanocrystals arranged along the Al-SBA-15 wall direction and formed a new ordered mesostrcuture. In addition, the Beta nanocrystal aggregates has another kind of large cavity that connected through the mesopores after the removal of carbonaceous particles. On the other hand, the high-quality framework assembly derived from the slow mass transfer directly caused strong acidity of the final Beta nanocrystal aggregates. The advanced acidic properties combined with the excellent hierarchical textural characteristic endow Beta nanocrystal aggregates with the great application potential in acid catalytic reactions involving large molecules.

Key words: Hierarchical Beta, Al-SBA-15, Seed-assisted steaming conversion, Framework assembly

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