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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.

该项目旨在以典型的方式开发用于乙醇脱氢的纳米结构催化剂。它依赖于载体和铜之间界面的可控形成和修饰作为活性相。这应该解决两个问题，解决方案从系统可用的知识开始。二氧化硅作为载体可以很好地稳定铜纳米颗粒，这是因为铜和载体之间形成了氧桥。另一方面，二氧化硅上的硅醇基团导致副反应，降低了乙醛的选择性。碳是一种副反应减少的替代载体，但铜颗粒只是弱锚定的，因此这样的系统容易烧结。这些问题应该通过设计的界面来解决。首先，二氧化硅将被覆盖一层薄薄的碳层，这将抑制副反应。然后，铜纳米颗粒将被沉积。氢气中的热处理会导致碳的局部甲烷化，这样铜颗粒就会穿过碳层移动到二氧化硅表面，在那里它们紧密地固定在那里。这样的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。第一种是以碳化硅为载体，通过控制处理可以对其表面进行不同类型的缺陷改性。铜可以固定在这些缺陷上，从而有效地固定，但由于与二氧化硅相比，表面功能不同，副反应可能会被抑制。第二个系统依赖于氧化物纳米管阵列，这是最近首次合成的。这些管子可以由直径在3纳米量级的氧化锆制成。在管子中，由于直径较小，铜纳米颗粒将被固定，氧原子靠近铜位。这与催化剂对乙醛的高选择性有关。催化剂在乙醇脱氢反应中的活性和选择性将得到表征。催化剂的性质将在非原位和反应条件下进行全面的表征，以便将定制的界面性质与催化性质相关联，从而进一步提高催化剂的性能。虽然工作的重点是标题反应，但将这些概念推广到其他系统是可能的。因此，希望这项研究将为以知识为基础的纳米结构催化剂的开发提供蓝图。