A bioscaffolding strategy for hierarchical zeolites with a nanotube-trimodal network.
A bioscaffolding strategy for hierarchical zeolites with a nanotube-trimodal network.
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具有纳米管三峰网络的分级沸石的生物支架策略
DOI：
10.1039/c5sc03837e
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发表时间：
2016-02-01
期刊：
影响因子：
8.4
通讯作者：
Xu R
中科院分区：
文献类型：
--
作者：
Li G;Huang H;Yu B;Wang Y;Tao J;Wei Y;Li S;Liu Z;Xu Y;Xu R
层次化的沸石海绵具有纳米管支架结构、纳米管-三模连接性和具有可调几何结构的自生成纳米管。具有多峰孔隙率的分级沸石整体非常重要，因为它们为高级应用开辟了新的领域。到目前为止，基于纳米管支架的分级沸石还没有报道。受生物矿物组织的启发，我们开发了一种新颖的前驱分子筛支架-固相结晶策略，具有独特的纳米管支架结构和纳米管-三模网络，其中生物分子自组装(BSA)提供了支架蓝图。通过气相处理的方法制备了分子筛MFI纳米管支架，在此过程中观察到了分段空洞和固体桥等演化现象，这与固相结晶体系中的Kirkendall效应一致。纳米管壁由相互生长的单晶组成，具有良好的机械稳定性。通过改变前驱层的厚度，纳米管的内径可以在30到90 nm之间调节。可以通过选择牛血清白蛋白来调节被交联型纳米管包裹的大孔。狭窄的介孔是由相互生长的纳米晶体形成的。与常规ZSM-5相比，具有纳米管(90 Nm)、微孔(0.55 nm)、中孔(2 Nm)和大孔(700 Nm)的层状ZSM-5整体在甲醇合成烃(MTH)反应中表现出更好的催化性能。BSA在晶化后保持不变，使沸石纳米管支架具有更高水平的组织化和功能化。目前的工作可能会为具有纳米管支架结构的分级沸石整体和纳米管-多模式网络提供一种通用的策略，从而获得自支撑和活性的沸石催化剂，以及更广泛的应用。
Hierarchical zeolite sponges with a nanotube scaffolding architecture, nanotube-trimodal connectivity and self-generated nanotubes with tunable geometry. Hierarchical zeolite monoliths with multimodal porosity are of paramount importance as they open up new horizons for advanced applications. So far, hierarchical zeolites based on nanotube scaffolds have never been reported. Inspired by the organization of biominerals, we have developed a novel precursor scaffolding-solid phase crystallization strategy for hierarchical zeolites with a unique nanotube scaffolding architecture and nanotube-trimodal network, where biomolecular self-assembly (BSA) provides a scaffolding blueprint. By vapor-treating Sil-1 seeded precursor scaffolds, zeolite MFI nanotube scaffolds are self-generated, during which evolution phenomena such as segmented voids and solid bridges are observed, in agreement with the Kirkendall effect in a solid-phase crystallization system. The nanotube walls are made of intergrown single crystals rendering good mechanical stability. The inner diameter of the nanotube is tunable between 30 and 90 nm by varying the thickness of the precursor layers. Macropores enclosed by cross-linked nanotubes can be modulated by the choice of BSA. Narrow mesopores are formed by intergrown nanocrystals. Hierarchical ZSM-5 monoliths with nanotube (90 nm), micropore (0.55 nm), mesopore (2 nm) and macropore (700 nm) exhibit superior catalytic performance in the methanol-to-hydrocarbon (MTH) conversion compared to conventional ZSM-5. BSA remains intact after crystallization, allowing a higher level of organization and functionalization of the zeolite nanotube scaffolds. The current work may afford a versatile strategy for hierarchical zeolite monoliths with nanotube scaffolding architectures and a nanotube-multimodal network leading to self-supporting and active zeolite catalysts, and for applications beyond.
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影响因子：
15
作者：
Groen, JC;Bach, T;Pérez-Ramírez, J
通讯作者：
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影响因子：
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