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An unprecedented c-oriented DDR@MWW zeolite hybrid membrane: new insights into H2-permselectivities via six membered-ring pores
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-07-03 , DOI: 10.1039/d0ta03892j Eunhee Jang 1, 2, 3, 4, 5 , Jeong Hyeon Lee 5, 6, 7, 8, 9 , Sungwon Hong 1, 2, 3, 4, 5 , Yanghwan Jeong 1, 2, 3, 4, 5 , Jin Chul Kim 5, 6, 7, 8, 9 , Dongjae Kim 5, 10, 11, 12 , Hionsuck Baik 4, 5, 13, 14 , Eunjoo Kim 1, 2, 3, 4, 5 , Nakwon Choi 5, 15, 16, 17, 18 , Jaewook Nam 5, 10, 11, 12, 19 , Sung June Cho 5, 20, 21, 22 , Sang Kyu Kwak 5, 6, 7, 8, 9 , Jungkyu Choi 1, 2, 3, 4, 5
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-07-03 , DOI: 10.1039/d0ta03892j Eunhee Jang 1, 2, 3, 4, 5 , Jeong Hyeon Lee 5, 6, 7, 8, 9 , Sungwon Hong 1, 2, 3, 4, 5 , Yanghwan Jeong 1, 2, 3, 4, 5 , Jin Chul Kim 5, 6, 7, 8, 9 , Dongjae Kim 5, 10, 11, 12 , Hionsuck Baik 4, 5, 13, 14 , Eunjoo Kim 1, 2, 3, 4, 5 , Nakwon Choi 5, 15, 16, 17, 18 , Jaewook Nam 5, 10, 11, 12, 19 , Sung June Cho 5, 20, 21, 22 , Sang Kyu Kwak 5, 6, 7, 8, 9 , Jungkyu Choi 1, 2, 3, 4, 5
Affiliation
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Despite the success of several types of homogeneous zeolite membranes, the manufacturing based on only one type of zeolite largely limits the flexible, reliable synthetic route toward the formation of continuous zeolite membranes. Herein, we demonstrate heterogeneous epitaxial growth of a seed layer using two structurally compatible zeolites. Specifically, MCM-22 (MWW type zeolites) seed layers were epitaxially grown with a synthetic precursor that leads to the DDR type zeolite. The resulting heterogeneous films, referred to as DDR@MWW hybrid films, were continuously formed on porous supports. Furthermore, heteroepitaxial growth of the c-oriented MCM-22 seed layer yielded a preferential c-out-of-plane orientation; accordingly, six membered-ring (6-MR) pores (having a maximum size of ∼0.28 nm) along the c-axis of the MWW and DDR zeolites were, for the first time, aligned in the out-of-plane direction. Subsequently, this good model sample was adopted for determining the H2-permselectivities of the 6-MR pores; surprisingly, the 6-MR pores were rather impermeable to both H2 and CO2 molecules up to ∼200 °C so that the c-oriented hybrid membrane exhibited modest CO2-permselectivities over N2 (0.364 nm) or CH4 (0.38 nm) at the expense of reduced CO2 molar flux. Lastly, this experimental observation was further complemented with rigorous molecular dynamics simulations on well-designed DDR zeolite membranes.
中文翻译：
前所未有的c定向DDR @ MWW沸石杂化膜：通过6个成员环孔对H2渗透性的新见解
尽管几种类型的均质沸石膜都取得了成功，但是仅基于一种类型的沸石的制造在很大程度上限制了形成连续沸石膜的柔性，可靠的合成途径。在本文中，我们展示了使用两种结构相容的沸石进行种子层的异质外延生长。具体而言，用合成的前驱体外延生长MCM-22（MWW型沸石）晶种层，从而形成DDR型沸石。所得的异质膜（称为DDR @ MWW混合膜）在多孔载体上连续形成。此外，c取向MCM-22种子层的异质外延生长产生了优先的c面外定向；因此，沿着MWW和DDR沸石c轴的六个成员环（6-MR）孔（最大尺寸为〜0.28 nm）首次在面外方向排列。随后，采用这种良好的模型样品来确定6-MR孔的H 2-渗透选择性。令人惊讶的是，在约200°C的温度下，6-MR孔对H 2和CO 2分子均不可渗透，因此c取向杂化膜在N 2（0.364 nm）或CH 4（0.38 ）上表现出适度的CO 2渗透选择性。nm）的代价是减少了CO 2摩尔通量。最后，在精心设计的DDR沸石膜上，通过严格的分子动力学模拟进一步补充了该实验观察结果。
更新日期：2020-07-21
中文翻译：
前所未有的c定向DDR @ MWW沸石杂化膜：通过6个成员环孔对H2渗透性的新见解
尽管几种类型的均质沸石膜都取得了成功，但是仅基于一种类型的沸石的制造在很大程度上限制了形成连续沸石膜的柔性，可靠的合成途径。在本文中，我们展示了使用两种结构相容的沸石进行种子层的异质外延生长。具体而言，用合成的前驱体外延生长MCM-22（MWW型沸石）晶种层，从而形成DDR型沸石。所得的异质膜（称为DDR @ MWW混合膜）在多孔载体上连续形成。此外，c取向MCM-22种子层的异质外延生长产生了优先的c面外定向；因此，沿着MWW和DDR沸石c轴的六个成员环（6-MR）孔（最大尺寸为〜0.28 nm）首次在面外方向排列。随后，采用这种良好的模型样品来确定6-MR孔的H 2-渗透选择性。令人惊讶的是，在约200°C的温度下，6-MR孔对H 2和CO 2分子均不可渗透，因此c取向杂化膜在N 2（0.364 nm）或CH 4（0.38 ）上表现出适度的CO 2渗透选择性。nm）的代价是减少了CO 2摩尔通量。最后，在精心设计的DDR沸石膜上，通过严格的分子动力学模拟进一步补充了该实验观察结果。
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