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Novel nanostructured catalysts for the high-temperature electro-oxidation of small organic molecules

用于有机小分子高温电氧化的新型纳米结构催化剂

基本信息

批准号：
164152250
负责人：
Professor Dr. Rolf Jürgen Behm
金额：
--
依托单位：
Institut für Theoretische Chemie
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2010
资助国家：
德国
起止时间：
2009-12-31 至 2013-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/164152250?language=en
关键词：
Novel nanostructured catalysts temperature electro

项目摘要

We aim at an in-depth understanding of i) the structure-reactivity correlation in platinum metal (Pt, Pd, ...) nanoparticles, using nanoparticles with well defined and variable shape and facet orientation, and of ii) the surface composition of shape-defined bimetallic nanoparticles in the oxidation of small organic molecules (formic acid, methanol, ethanol …). In addition to understanding the molecular scale reaction mechanism on nanoparticles of well defined morphology and structure, and the effect of surface structure and composition, we are particularly interested in effects caused by the reaction conditions (concentration, temperatures), covering a wide range of reaction conditions, up to fuel cell relevant reaction and transport conditions. Based on the resulting mechanistic understanding, we aim at a systematic improvement of the catalytic behavior of these nanoparticle catalysts in the oxidation of small organic molecules. Furthermore, we will elucidate the stability of the pre-shaped nanoparticles with respect to shape relaxation and sintering, which will be crucial for applications.These objectives shall be reached using preferentially oriented nanoparticles with diameters in the 5-10 nm range and different shapes, whose size and shape will be varied in a controlled way. Synthesis of the nanoparticles and its further systematic improvement is an important part of the project. Variations in the nanoparticle shape correspond to changes in the surface structure, due to the facet specific surface structure. The mechanistic interpretation will largely be based on combined electrochemical and in-situ spectroscopic measurements (Differential Electrochemical Mass Spectrometry (DEMS) and ATR-FTIR), which are performed under up to fuel cell relevant reaction conditions. They provide detailed information on the nature and role of adsorbed and volatile reaction intermediates and reaction side products. Furthermore, we will make use of existing experimental and theoretical data and mechanistic proposals for the respective reactions, and of results in collaborating theory groups.

我们的目标是深入了解i）铂金属（Pt，Pd，.）纳米颗粒，使用具有良好定义的和可变的形状和小面取向的纳米颗粒，和ii）在小有机分子（甲酸、甲醇、乙醇.）的氧化中形状定义的纳米颗粒的表面组成。除了了解纳米颗粒的分子尺度反应机制以及表面结构和组成的影响外，我们对反应条件（浓度，温度）引起的影响特别感兴趣，涵盖广泛的反应条件，直到燃料电池相关的反应和运输条件。基于由此产生的机制的理解，我们的目标是在这些纳米粒子催化剂的催化行为的系统改进，在有机小分子的氧化。此外，我们将阐明预成型纳米粒子的形状弛豫和烧结方面的稳定性，这将是至关重要的应用。这些目标应达到使用优先取向的纳米粒子的直径在5-10 nm范围内和不同的形状，其大小和形状将在一个控制的方式变化。纳米粒子的合成及其进一步的系统改进是该项目的重要组成部分。由于小面特定的表面结构，纳米颗粒形状的变化对应于表面结构的变化。机理解释将主要基于组合的电化学和原位光谱测量（差分电化学质谱（DEMS）和ATR-FTIR），其在燃料电池相关反应条件下进行。它们提供了关于吸附和挥发性反应中间体和反应副产物的性质和作用的详细信息。此外，我们将利用现有的实验和理论数据和机制的建议，为各自的反应，并在合作的理论小组的结果。