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首页> 外文期刊>Advanced Materials >Engineering of Microcage Carbon Nanotube Architectures with Decoupled Multimodal Porosity and Amplified Catalytic Performance
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Engineering of Microcage Carbon Nanotube Architectures with Decoupled Multimodal Porosity and Amplified Catalytic Performance

机译：微量碳纳米管架构与去耦多式孔隙度和扩增催化性能的工程

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摘要

New approaches for the engineering of the 3D microstructure, pore modality, and chemical functionality of hierarchically porous nanocarbon assemblies are key to develop the next generation of functional aerogel and membrane materials. Here, interfacially driven assembly of carbon nanotubes (CNT) is exploited to fabricate structurally directed aerogels with highly controlled internal architectures, composed of pseudo-monolayer, CNT microcages. CNT Pickering emulsions enable engineering at fundamentally different length scales, whereby the microporosity, mesoporosity, and macroporosity are decoupled and individually controlled through CNT type, CNT number density, and process energy, respectively. In addition, metal nanocatalysts (Cu, Pd, and Ru) are embedded within the architectures through an elegant sublimation and shock-decomposition approach; introducing the first approach that enables through-volume functionalization of intricate, pre-designed aerogels without microstructural degradation. Catalytic structure-function relationships are explored in a pharma-important amidation reaction; providing insights on how the engineered frameworks enhance catalyst activity. A sophisticated array of advanced tomographic, spectroscopic, and microscopic techniques reveal an intricate 3D assembly of CNT building-blocks and their influence on the functional properties of the enhanced nanocatalysts. These advances set a basis to modulate structure and chemistry of functional aerogel materials independently in a controlled fashion for a variety of applications, including energy conversion and storage, smart electronics, and (electro)catalysis.
机译：分层多孔纳米碳组合物的3D微结构，孔隙态和化学功能的新方法是开发下一代功能气体和膜材料的关键。这里，碳纳米管（CNT）的界面驱动的组装被利用以制造具有高度受控的内部架构的结构上定向的气凝胶，由伪单层，CNT显微量组成。 CNT皮克林乳液在基本上不同的长度尺度可以实现工程，从而分别通过CNT型，CNT数密度和工艺能量分离和单独控制微孔率，中渗透性和巨孔率。此外，通过优雅的升华和冲击分解方法嵌入建筑内的金属纳米催化剂（Cu，Pd和Ru）;介绍了一种能够通过微观结构降解的复杂的复杂的经济体积官能化的第一种方法。催化结构功能关系在药物重要的酰胺化反应中探讨;提供关于工程框架如何增强催化剂活动的见解。一种复杂的一系列先进断层，光谱和微观技术揭示了CNT构建块的复杂3D组装及其对增强型纳米催化剂的功能性质的影响。这些进步设定了一种基础，可在各种应用中独立地调节功能性气凝胶材料的结构和化学，包括各种应用，包括能量转换和储存，智能电子和（电）催化。

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