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Interfacial design of function integrated catalysts for ethanol dehydrogenation

乙醇脱氢功能集成催化剂的界面设计

基本信息

批准号：
323224195
负责人：
Professor Dr. Ferdi Schüth
金额：
--
依托单位：
Max-Planck-Institut für Kohlenforschung
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2017
资助国家：
德国
起止时间：
2016-12-31 至 2020-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/323224195?language=en
关键词：
Interfacial design function integrated catalysts

项目摘要

The project aims in a prototypical manner at the development of nanostructured catalysts for the dehydrogenation of ethanol. It relies on controlled formation and modification of interfaces between support and copper as the active phase. This should solve two problems, with the solution starting from the knowledge available for the system. Silica as support stabilizes copper nanoparticles very well, due to the formation of oxobridges between copper and support. On the other hand, silanol groups on the silica lead to side reaction, which reduce the selectivity to acetaldehyde. Carbon is an alternative support with reduced side reactions, but the copper particles are only weakly anchored, so that such systems are susceptible to sintering.These problems shall be solved by a designed interface. First, silica will be coated with a thin carbon layer, which suppresses the side reactions. Then copper nanoparticles will be deposited. Thermal treatement in hydrogen leads to local methanization of the carbon, so that the copper particles move through the carbon layer to the silica surface, where they are tightly anchored.Such catalysts are probably not easy to regenerate, since oxidative treatment will destroy the carbon layer. Therefore, two alternative concepts shall also be studied. The first uses SiC as support, the surface of which can be modified with different types of defects by controlled treatment. Copper can be anchored to these defects and thus efficiently immobilized, but due to the different surface functionalities compared to silica, side reactions may possibly be suppressed. The second system relies on arrays of oxide nanotubes, which have recently been synthesized for the first time. These tubes can be made from zirconia, with diameters on the order of 3 nm. In the tubes, copper nanoparticles will be immobilized, with the oxygen atoms being close to the copper sites, due to the small diameters. This is connected with high acetaldehyde selectivity of the catalyst.The catalysts will be characterized in ethanol dehydrogenation with respect to activity and selectivity. The properties of the catalysts will comprehensively be characterized ex-situ and under reaction conditions in order to correlate the tailored interface properties to the catalytic properties, which serves to improve the catalysts further.While the work is focussed on the title reaction, it will probably be possible to generalize the concepts to be developed to other systems. It is therefore hoped that the study will provide a blueprint for the knowledge-based development of nanostructured catalysts.

该项目旨在以原型方式开发用于乙醇脱氢的纳米结构催化剂。它依赖于载体和作为活性相的铜之间的界面的受控形成和改性。这应该解决两个问题，解决方案从系统可用的知识开始。二氧化硅作为载体非常好地稳定了铜纳米颗粒，这是由于在铜和载体之间形成氧桥。另一方面，二氧化硅上的硅烷醇基团导致副反应，这降低了乙醛的选择性。碳是一种副反应减少的替代载体，但铜颗粒的锚定作用很弱，因此这种系统容易烧结。这些问题应通过设计界面来解决。首先，二氧化硅将被覆盖一层薄碳层，这抑制了副反应。然后将沉积铜纳米颗粒。在氢气中的热分解导致碳的局部甲烷化，因此铜颗粒穿过碳层移动到二氧化硅表面，在那里它们被紧紧地固定住。这种催化剂可能不容易再生，因为氧化处理会破坏碳层。因此，还应研究两个备选概念。第一种方法使用SiC作为载体，其表面可以通过控制处理用不同类型的缺陷进行改性。铜可以锚定到这些缺陷上，从而有效地固定，但由于与二氧化硅相比不同的表面官能度，可能会抑制副反应。第二个系统依赖于氧化物纳米管阵列，这是最近首次合成。这些管可以由氧化锆制成，直径约为3nm。在管中，铜纳米颗粒将被固定，由于直径小，氧原子靠近铜位点。这与催化剂的高乙醛选择性有关。该催化剂将在乙醇脱氢的活性和选择性方面进行表征。催化剂的性能将全面表征异位和反应条件下，以关联定制的界面性能的催化性能，这有助于进一步提高催化剂，虽然工作集中在标题反应，它可能会推广的概念，以开发其他系统。因此，希望这项研究将提供一个蓝图，以知识为基础的纳米结构催化剂的发展。