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金属-氧化物型纳米异质结构可能存在界面间的电子和物质传输,因而导致性能的提升,目前得到广泛的关注.对于这类金属-氧化物型纳米异质结构在催化反应中的结构-效能关系,以往的研究存在以下不足之处:一方面对于尺寸的控制还有欠缺,不能合成尺寸可控的单分散样品;另一方面,对催化剂电子结构的表征主要停留在真空或气相环境,而液相原位表征方法亟待发展.本研究工作发展了一种甲酰胺溶剂合成体系,可以尺寸连续可调地合成一系列钯-氧化铁纳米异质结构和单独的钯纳米晶.利用这些模型催化剂,结合液相电化学测试方法,我们原位研究了它们的电子结构,并发现在真空和液相环境中,这些催化剂的电子结构有明显差异.这表明传统的真空表征方法可能会造成与真实构效关系的偏离.本研究表明,高质量的模型催化剂和原位表征方法对于研究构效关系都是至关重要的.这对于发展高效的金属-氧化物型液-固异相催化剂具有一定的启示意义.
Metal-oxide nano-heterostructures are likely to exist between the interface of the electron and material transport, thus leading to performance improvement, has been widely concerned.For such metal-oxide nano-heterostructures in the catalytic reaction structure - The previous studies have the following shortcomings: on the one hand, the control of the size is not enough, and the monodisperse samples with controlled size can not be synthesized; on the other hand, the characterization of the catalyst electronic structure mainly stays in the vacuum or gas phase environment, However, the in-situ liquid-phase characterization method needs to be developed urgently.In this work, a formamide solvent synthesis system was developed to synthesize a series of palladium-iron oxide nano-heterostructures and palladium nano-crystals with continuous and adjustable size.Using these models Catalysts, in combination with liquid-phase electrochemical tests, we investigated their electronic structures in situ and found that there was a clear difference in the electronic structure of these catalysts in both vacuum and liquid environments, suggesting that conventional vacuum characterization methods may result in a Structure-activity relationship deviation.This study shows that high-quality model catalysts and in situ characterization methods for the study of the structure-activity relationship are This is crucial for the development of efficient metal - having a certain significance inspiration solid heterogeneous catalyst - oxide solution.