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Complex bifunctional metal nanostructures for in situ monitoring of nanoparticle-catalyzed reactions by surface-enhanced Raman spectroscopy

通过表面增强拉曼光谱原位监测纳米粒子催化反应的复杂双功能金属纳米结构

基本信息

批准号：
228269688
负责人：
Professor Dr. Wei Xie
金额：
--
依托单位：
Nankai University
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2012
资助国家：
德国
起止时间：
2011-12-31 至 2014-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/228269688?language=en
关键词：
Complex bifunctional metal nanostructures situ

项目摘要

In situ monitoring of heterogeneously catalyzed reactions requires interface/surface-selective techniques. Surface-enhanced Raman spectroscopy (SERS) provides molecular structural information on chemical species adsorbed onto the surface of plasmonic nanostructures such as noble metal nanoparticles. SERS and catalysis have no direct topical overlap in terms of nanoparticle functionalities since plasmonic/SERS and catalytic properties are usually disjunct. Therefore, applications of colloidal SERS in heterogeneous catalysis are currently rare, despite the wealth of chemical information accessible by vibrational spectroscopy. In order to overcome the limited use of SERS in heterogeneous catalysis, bifunctional metal nanostructures with catalysts inside the localized surface plasmon resonance field of the plasmonic metal are required. The central aim of this proposal is to design and synthesize tailor-made bifunctional metal colloids with both plasmonic/SERS and catalytic activities for in situ monitoring of nanoparticle-catalyzed reactions. Complex metal superstructures comprising a silica shell-isolated SERS-active core and catalytically active satellite particles assembled onto the core as well as bifunctional hybrid nanoparticles will be synthesized and analyzed with respect to their SERS and catalytic activities. Computational simulations will be performed in order to understand and predict the plasmonic properties of the bifunctional nanostructures. SERS monitoring of model reactions will be carried out by using microfluidic devices to study the kinetics of heterogeneous catalysis on the surface of the bifunctional nanostructures. Experimental SERS spectra will be analyzed with multivariate methods to obtain quantitative information on the involved chemical species and molecular changes during the catalytic reaction. For expanding this approach to molecules without surface-seeking groups, the bifunctional nanostructures will be coated for either capturing or enriching the involved species near the metal surface. Finally, via investigations at the single-particle level, we aim at establishing fundamental correlations between the morphology of a bifunctional nanostructure and both its catalytic and plasmonic/SERS activities.

多相催化反应的原位监测需要界面/表面选择性技术。表面增强拉曼光谱（Sers）提供了关于吸附到等离子体纳米结构（例如贵金属纳米颗粒）表面上的化学物质的分子结构信息。Sers和催化在纳米颗粒功能方面没有直接的局部重叠，因为等离子体/Sers和催化性质通常是分离的。因此，胶体Sers在多相催化中的应用目前是罕见的，尽管丰富的化学信息可通过振动光谱。为了克服Sers在非均相催化中的有限应用，需要在等离子体金属的局部表面等离子体共振场中具有催化剂的双功能金属纳米结构。该提案的中心目标是设计和合成定制的双功能金属胶体，其具有等离子体/Sers和催化活性，用于原位监测纳米颗粒催化的反应。将合成包含二氧化硅壳隔离的SERS活性核和组装到核上的催化活性卫星颗粒以及双功能混合纳米颗粒的复合金属超结构，并分析它们的Sers和催化活性。为了理解和预测双功能纳米结构的等离子体性质，将进行计算模拟。Sers监测模型反应将通过使用微流控装置进行，以研究双功能纳米结构表面上的非均相催化的动力学。实验Sers光谱将用多元方法分析，以获得催化反应过程中所涉及的化学物种和分子变化的定量信息。为了将这种方法扩展到没有表面寻求基团的分子，双功能纳米结构将被涂覆以捕获或富集金属表面附近的相关物质。最后，通过在单粒子水平上的调查，我们的目标是建立一个双功能纳米结构的形态和它的催化和等离子体/Sers活性之间的基本相关性。