TY - JOUR
T1 - A stable zeolite with atomically ordered and interconnected mesopore channel
AU - Lu, Peng
AU - Xu, Jiaoyan
AU - Sun, Yiqing
AU - Guillet-Nicolas, Rémy
AU - Willhammar, Tom
AU - Fahda, Mohammad
AU - Dib, Eddy
AU - Wang, Bo
AU - Qin, Zhengxing
AU - Xu, Hongyi
AU - Cho, Jung
AU - Liu, Zhaopeng
AU - Yu, Haijun
AU - Yang, Xiaobo
AU - Lang, Qiaolin
AU - Mintova, Svetlana
AU - Zou, Xiaodong
AU - Valtchev, Valentin
N1 - © The Author(s) 2024.
PY - 2024/12/12
Y1 - 2024/12/12
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85211643707&partnerID=8YFLogxK
U2 - 10.1038/s41586-024-08206-1
DO - 10.1038/s41586-024-08206-1
M3 - Article
C2 - 39663489
AN - SCOPUS:85211643707
SN - 0028-0836
VL - 636
SP - 368
EP - 373
JO - Nature
JF - Nature
IS - 8042
M1 - 3152
ER -