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用于低温氨氧化的铜-钌纳米颗粒催化剂的自下而上设计。

Bottom-Up Design of a Copper-Ruthenium Nanoparticulate Catalyst for Low-Temperature Ammonia Oxidation.

机构信息

SurfCat, Department of Physics, Technical University of Denmark, Fysikvej, Building 311, 2800, Kgs. Lyngby, Denmark.

Center for Electron Nanoscopy, Technical University of Denmark, Fysikvej, Building 307, 2800, Kgs. Lyngby, Denmark.

出版信息

Angew Chem Int Ed Engl. 2017 Jul 17;56(30):8711-8715. doi: 10.1002/anie.201703468. Epub 2017 Jun 14.

Abstract

A novel nanoparticulate catalyst of copper (Cu) and ruthenium (Ru) was designed for low-temperature ammonia oxidation at near-stoichiometric mixtures using a bottom-up approach. A synergistic effect of the two metals was found. An optimum CuRu catalyst presents a reaction rate threefold higher than that for Ru and forty-fold higher than that for Cu. X-ray absorption spectroscopy suggests that in the most active catalyst Cu forms one or two monolayer thick patches on Ru and the catalysts are less active once 3D Cu islands form. The good performance of the tuned Cu/Ru catalyst is attributed to changes in the electronic structure, and thus the altered adsorption properties of the surface Cu sites.

摘要

采用自下而上的方法设计了一种新型的铜(Cu)和钌(Ru)纳米颗粒催化剂,用于在接近化学计量比的混合物中低温催化氨氧化反应。研究发现两种金属具有协同作用。最佳的 CuRu 催化剂的反应速率比 Ru 高三倍,比 Cu 高四十倍。X 射线吸收光谱表明,在最活跃的催化剂中,Cu 在 Ru 上形成一层或两层单原子厚的薄片,一旦形成 3D Cu 岛,催化剂的活性就会降低。经过调整的 Cu/Ru 催化剂具有良好的性能,这归因于其电子结构的变化,以及表面 Cu 位吸附性能的改变。

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