Study on In Situ Characterization of Metal-Support Interaction and Correlative Structure-Reactivity Relationship in Catalysis

催化中金属-载体相互作用及相关结构-反应性关系的原位表征研究

• 批准号: 392178740
• 负责人: Dr. Yuemin Wang
• 金额: --
• 依托单位: Dalian Institute of Chemical Physics
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2018
• 资助国家: 德国
• 起止时间: 2017-12-31 至 2020-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/392178740?language=en
• 关键词: Study; Situ; Characterization; Metal; Support

The study on ceria-supported IB metal (Au, Cu, Ag) nanoparticles (NPs) with different size and morphologies has become one of the most interesting topics in heterogeneous catalysis due to the extraordinary catalytic activities for many important reactions. The strong metal-support interaction (SMSI) has long been known to play a key role in the catalytic performance (activity, selectivity and stability) of oxide-supported metal catalysts. Despite extensive investigations, a fundamental understanding of the SMSI effect and the structure-activity relationship of metal/ceria catalysts is still lacking and many crucial issues remain unanswered. This is primarily due to the great complexity of nanostructured metal/ceria materials and the lack of a thorough surface science study on well-defined model catalysts. In this joint project, the two partner groups will work in a very close collaboration on fabrication and in-situ state-of-the-art spectroscopic and microscopic characterization of metal/ceria systems. The German partner will carry out a thorough spectroscopic (UHV-FTIRS in conjunction with XPS and NEXAFS) study on IB metal (Cu, Ag, Au) clusters dispersed on ceria surfaces of both single crystals (polarization-dependent IRRAS) and nanostructured materials (IR transmission). The Chinese partner will focus on the synthesis of different types of metal/ceria nanoparticles with tunable size and shape. The corresponding ETEM/STEM-Nanoreactor experiments will be conducted to image the dynamic behavior of various metal/ceria catalysts under activation and reaction conditions. In addition, we will do systematic and collaborative work on reaction mechanisms and reaction kinetics of selected reactions such as low-temperature CO oxidation and water gas shift reactions. We aim to achieve detailed insight into the structural, electronic and reactive properties of the complex nanostructured metal/oxide catalysts based on reliable and comprehensive reference data acquired for different metal/oxide monocrystal model systems. The overarching objective is an atomic-level understanding of the SMSI effect and the intrinsic structure-reactivity relationship, which enables the predictive, rational design of ceria-based catalytic materials at the nanoscale.

不同尺寸和形貌的氧化铈负载IB金属（Au，Cu，Ag）纳米粒子（NPs）由于对许多重要反应具有优异的催化活性而成为多相催化领域的研究热点之一。强金属-载体相互作用（SMSI）在氧化物负载的金属催化剂的催化性能（活性、选择性和稳定性）中起着关键作用。尽管进行了广泛的研究，但对金属/氧化铈催化剂的SMSI效应和结构-活性关系的基本理解仍然缺乏，许多关键问题仍然没有答案。这主要是由于纳米结构的金属/氧化铈材料的高度复杂性和缺乏对明确定义的模型催化剂进行彻底的表面科学研究。在这个联合项目中，两个合作伙伴小组将在金属/二氧化铈系统的制造和原位最先进的光谱和显微表征方面进行非常密切的合作。德国合作伙伴将对分散在单晶（偏振依赖IRRAS）和纳米结构材料（IR透射）的二氧化铈表面上的IB金属（Cu、Ag、Au）簇进行全面的光谱（UHV-FTIRS结合XPS和NEXAFS）研究。中国合作伙伴将专注于合成不同类型的金属/二氧化铈纳米颗粒，其尺寸和形状可调。将进行相应的ETEM/STEM纳米反应器实验，以成像各种金属/氧化铈催化剂在活化和反应条件下的动态行为。此外，我们将对选定的反应，如低温CO氧化和水煤气变换反应的反应机理和反应动力学进行系统和协作工作。我们的目标是实现详细的洞察复杂的纳米结构的金属/氧化物催化剂的结构，电子和反应特性的基础上获得的可靠和全面的参考数据为不同的金属/氧化物单晶模型系统。总体目标是对SMSI效应和内在结构-反应性关系的原子级理解，这使得能够预测纳米级氧化铈基催化材料的合理设计。