法国鲁昂大学Valtchev, Valentin研究团队报道了一种具有原子有序互联介孔通道的稳定沸石。相关研究成果发表在2024年12月11日出版的《自然》。

沸石是由共角四面体（SiO₄和AlO₄）构成的结晶微孔材料，在工业上有许多应用，如离子交换剂、吸附剂和非均相催化剂。然而，微孔的存在阻碍了沸石在处理大块基材的领域的使用。在沸石中引入外源性介孔，即晶间/晶内介孔，是克服扩散障碍的解决方案。

然而，这些外在的中孔通常是无序和不均匀的。此外，酸度和结晶度总是在一定程度上受到影响。因此，合成具有均匀尺寸且与微孔晶体连接的具有固有中孔的热稳定沸石是非常需要的，但尚未实现。

ZMQ-1是一种铝硅酸盐沸石，具有由28×10×10环界定的交叉内孔-微孔通道系统，其中28环的自由直径为22.76×11.83，达到中孔域。具有Si/Al摩尔比可调框架的ZMQ-1具有高热稳定性和水热稳定性。ZMQ-1是第一个具有内在中微孔通道系统的铝硅酸盐沸石。

ZMQ-1的布朗斯特酸性赋予了，其在重油催化裂化中的高活性和独特的选择性。研究根据三维电子衍射（3DED）数据，确定了用于ZMQ-1合成的有机结构导向剂（OSDA）的位置，这表明了OSDA在形成本征介孔-微孔沸石中的独特结构导向作用。

该研究为制备其他稳定的含中孔沸石提供了动力。

附：英文原文

Title: A stable zeolite with atomically ordered and interconnected mesopore channel

Author: Lu, Peng, Xu, Jiaoyan, Sun, Yiqing, Guillet-Nicolas, Rmy, Willhammar, Tom, Fahda, Mohammad, Dib, Eddy, Wang, Bo, Qin, Zhengxing, Xu, Hongyi, Cho, Jung, Liu, Zhaopeng, Yu, Haijun, Yang, Xiaobo, Lang, Qiaolin, Mintova, Svetlana, Zou, Xiaodong, Valtchev, Valentin

Issue&Volume: 2024-12-11

Abstract: Zeolites are crystalline microporous materials constructed by corner-sharing tetrahedra (SiO4 and AlO4), with many industrial applications as ion exchangers, adsorbents and heterogeneous catalysts1,2,3,4. However, the presence of micropores impedes the use of zeolites in areas dealing with bulky substrates. Introducing extrinsic mesopores, that is, intercrystal/intracrystal mesopores, in zeolites is a solution to overcome the diffusion barrier5,6,7,8. Still, those extrinsic mesopores are generally disordered and non-uniform; moreover, acidity and crystallinity are always, to some extent, impaired9. Thus, synthesizing thermally stable zeolites with intrinsic mesopores that are of uniform size and crystallographically connected with micropores, denoted here as intrinsic mesoporous zeolite, is highly desired but still not achieved. Here we report ZMQ-1 (Zeolitic Materials, Qingdao Institute of Bioenergy and Bioprocess Technology, no. 1), an aluminosilicate zeolite with an intersecting intrinsic meso-microporous channel system delimited by 28×10× 10-rings, in which the 28-ring has a free diameter of 22.76×11.83, which reaches the mesopore domain. ZMQ-1 has high thermal and hydrothermal stability with tunable framework Si/Al molar ratios. ZMQ-1 is the first aluminosilicate zeolite with an intrinsic meso-microporous channel system. The Brnsted acidity of ZMQ-1 imparts high activity and unique selectivity in the catalytic cracking of heavy oil. The position of the organic structure-directing agent (OSDA) used for ZMQ-1 synthesis was determined from three-dimensional electron diffraction (3DED) data, which shows the unique structure-directing role of the OSDA in the formation of the intrinsic meso-microporous zeolite. This provides an incentive for preparing other stable mesopore-containing zeolites.

DOI: 10.1038/s41586-024-08206-1

Source: https://www.nature.com/articles/s41586-024-08206-1