Center for Catalytic Science and Technology, Department of Chemical Engineering, University of Delaware, Newark, Delaware 19716, USA.
Nat Chem. 2010 Jun;2(6):484-9. doi: 10.1038/nchem.626. Epub 2010 Apr 25.
The facile decomposition of ammonia to produce hydrogen is critical to its use as a hydrogen storage medium in a hydrogen economy, and although ruthenium shows good activity for catalysing this process, its expense and scarcity are prohibitive to large-scale commercialization. The need to develop alternative catalysts has been addressed here, using microkinetic modelling combined with density functional studies to identify suitable monolayer bimetallic (surface or subsurface) catalysts based on nitrogen binding energies. The Ni-Pt-Pt(111) surface, with one monolayer of Ni atoms residing on a Pt(111) substrate, was predicted to be a catalytically active surface. This was verified using temperature-programmed desorption and high-resolution electron energy loss spectroscopy experiments. The results reported here provide a framework for complex catalyst discovery. They also demonstrate the critical importance of combining theoretical and experimental approaches for identifying desirable monolayer bimetallic systems when the surface properties are not a linear function of the parent metals.
氨的简易分解对于将其作为氢能经济中的储氢介质非常关键。尽管钌对催化这一过程具有良好的活性，但由于其昂贵和稀缺，限制了其在大规模商业化中的应用。因此，需要开发替代催化剂。本研究采用微动力学建模结合密度泛函研究，根据氮结合能确定合适的基于单层双金属（表面或次表面）的催化剂。预测镍-铂-铂（111）表面（一层镍原子位于铂（111）基底上）是一种具有催化活性的表面。这通过程序升温脱附和高分辨率电子能量损失光谱实验得到了验证。这里报道的结果为复杂催化剂的发现提供了一个框架。它们还表明，当表面性质不是母体金属的线性函数时，结合理论和实验方法来识别理想的单层双金属体系至关重要。
