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具有12×10×7环通道的多维准沸石表现出高热稳定性和良好的气体吸附选择性。

A multi-dimensional quasi-zeolite with 12 × 10 × 7-ring channels demonstrates high thermal stability and good gas adsorption selectivity.

作者信息

Liang Jie, Xia Wei, Sun Junliang, Su Jie, Dou Maofeng, Zou Ruqiang, Liao Fuhui, Wang Yingxia, Lin Jianhua

机构信息

College of Chemistry and Molecular Engineering , Peking University , Beijing , 100871 , China . Email:

Berzelii Center EXSELENT on Porous Materials and Inorganic and Structural Chemistry , Department of Materials and Environmental Chemistry , Stockholm University , Stockholm , 10691 , Sweden.

出版信息

Chem Sci. 2016 May 1;7(5):3025-3030. doi: 10.1039/c5sc04916d. Epub 2016 Jan 25.

DOI:10.1039/c5sc04916d
PMID:29997792
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6005135/
Abstract

A novel quasi-zeolite PKU-15, with a rare 3-dimensional structure containing interconnected large (12-ring), medium (10-ring) and small (7-ring) multi-pore channels, was hydrothermally synthesised and characterised. A unique tri-bridging O anion is found to be encapsulated in the cage-like (Ge,Si)O building unit and energetically stabilises the PKU-15 framework. The removal of this oxygen atom would convert PKU-15 into a hypothetical zeolite PKU-15H. Thus, PKU-15 can be considered as a unique 'quasi-zeolite', which bridges porous germanates and zeolites. Owing to the absence of terminal Ge-OH groups in its structure, PKU-15 shows a remarkably high thermal stability of up to 600 °C. PKU-15 is also the first microporous germanate that exhibits permanent porosity, with a BET area of 428 m g and a good adsorption affinity toward CO.

摘要

一种新型的准沸石PKU - 15通过水热合成法制备并进行了表征,它具有罕见的三维结构,包含相互连接的大孔(12元环)、中孔(10元环)和小孔(7元环)多孔隙通道。研究发现一种独特的三桥连O阴离子被包裹在笼状的(Ge,Si)O构筑单元中,并在能量上稳定了PKU - 15骨架。去除这个氧原子会将PKU - 15转化为一种假设的沸石PKU - 15H。因此,PKU - 15可被视为一种独特的“准沸石”,它架起了多孔锗酸盐和沸石之间的桥梁。由于其结构中不存在末端Ge - OH基团,PKU - 15表现出高达600℃的显著高热稳定性。PKU - 15也是第一种表现出永久孔隙率的微孔锗酸盐,其BET比表面积为428 m²/g,对CO具有良好的吸附亲和力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/1d5bb57fd2f7/c5sc04916d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/0ad1784e19f7/c5sc04916d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/8fa24033d568/c5sc04916d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/ea2c1d9a7b57/c5sc04916d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/6294a929adbf/c5sc04916d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/1d5bb57fd2f7/c5sc04916d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/0ad1784e19f7/c5sc04916d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/8fa24033d568/c5sc04916d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/ea2c1d9a7b57/c5sc04916d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/6294a929adbf/c5sc04916d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3fd4/6005135/1d5bb57fd2f7/c5sc04916d-f5.jpg

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本文引用的文献

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SSZ-23: An Odd Zeolite with Pore Openings of Seven and Nine Tetrahedral Atoms.SSZ-23:一种具有七元环和九元环孔口的奇特沸石。
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ITQ-54: a multi-dimensional extra-large pore zeolite with 20 × 14 × 12-ring channels.ITQ-54:一种具有20×14×12环通道的多维超大孔沸石。
Chem Sci. 2015 Jan 1;6(1):480-485. doi: 10.1039/c4sc02577f. Epub 2014 Oct 8.
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Recent advances in zeolite chemistry and catalysis.
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A Crystalline Mesoporous Germanate with 48-Ring Channels for CO₂ Separation.具有 48 元环通道的用于 CO₂ 分离的结晶介孔锗酸盐。
Angew Chem Int Ed Engl. 2015 Jun 15;54(25):7290-4. doi: 10.1002/anie.201501718. Epub 2015 May 4.
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A 3D 12-ring zeolite with ordered 4-ring vacancies occupied by (H2O)2 dimers.一种具有有序四元环空位且被(H₂O)₂二聚体占据的三维十二元环沸石。
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