当前位置: X-MOL 学术Nature › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
A stable zeolite with atomically ordered and interconnected mesopore channel
Nature ( IF 50.5 ) Pub Date : 2024-12-11 , DOI: 10.1038/s41586-024-08206-1
Peng Lu, Jiaoyan Xu, Yiqing Sun, Rémy Guillet-Nicolas, Tom Willhammar, Mohammad Fahda, Eddy Dib, Bo Wang, Zhengxing Qin, Hongyi Xu, Jung Cho, Zhaopeng Liu, Haijun Yu, Xiaobo Yang, Qiaolin Lang, Svetlana Mintova, Xiaodong Zou, Valentin Valtchev

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 Å × 11.83 Å, 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 Brønsted 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 (3D ED) 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.



中文翻译:


一种稳定的沸石,具有原子有序且互连的介孔通道



沸石是由角共享四面体(SiO4 和 AlO4)构建的结晶微孔材料,在工业上可用作离子交换剂、吸附剂和非均相催化剂1,2,3,4。然而,微孔的存在阻碍了沸石在处理大块基材的区域使用。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5,6,7,8。尽管如此,那些外源性介孔通常是无序且不均匀的;此外,酸度和结晶度总是在某种程度上受到损害9。因此,合成具有大小均匀且与微孔晶体学连接的本征介孔的热稳定沸石,此处表示为本征介孔沸石,是非常理想的,但仍未实现。在这里,我们报道了 ZMQ-1(青岛生物能源与过程研究所沸石材料,第 1 名),一种铝硅酸盐沸石,具有由 28 个× 10 个× 10 个环界定的相交本征内禀中微孔通道系统,其中 28 环的自由直径为 22.76 Å × 11.83 Å,到达中孔域。ZMQ-1 具有很高的热稳定性和水热稳定性,框架 Si/Al 摩尔比可调。ZMQ-1 是第一种具有本征介观微孔通道系统的铝硅酸盐沸石。ZMQ-1 的 Brønsted 酸性在重油催化裂化中赋予高活性和独特的选择性。 用于 ZMQ-1 合成的有机结构导向剂 (OSDA) 的位置由三维电子衍射 (3D ED) 数据确定,这表明 OSDA 在内征介孔微孔沸石的形成中具有独特的结构导向作用。这为制备其他稳定的含中孔沸石提供了动力。

更新日期:2024-12-12
down
wechat
bug