Gruzeł Grzegorz, Piekarz Przemysław, Pawlyta Mirosława, Donten Mikołaj, Parlinska-Wojtan Magdalena
Institute of Nuclear Physics Polish Academy of Sciences , PL-31342 Krakow , Poland.
Institute of Engineering Materials and Biomaterials , Silesian University of Technology 44-100 Gliwice , Poland.
ACS Appl Mater Interfaces. 2019 Jun 26;11(25):22352-22363. doi: 10.1021/acsami.9b04690. Epub 2019 Jun 13.
Pt-based nanoframes are one of the most promising catalysts for ethanol oxidation reaction in direct ethanol fuel cells. It is important to understand the mechanisms responsible for creating these hollow nanoframe-based catalysts. Herein, for the first time, Pt-skin PtRhNi rhombic dodecahedral nanoframes were decorated with small SnO nanoparticles and were used as an efficient catalyst for the ethanol oxidation reaction. Moreover, by combining the ex situ scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy observations at various stages of synthesis, along with density functional theory calculations, it was possible to track the synthesis route of solid rhombic dodecahedral PtRhNi nanoparticles, which are the precursors of PtRhNi nanoframes. After the chemical etching of the Ni core from solid PtRhNi nanoparticles, the obtained nanoframes were decorated with SnO nanoparticles. The resulting SnO@PtRhNi heteroaggregates were deposited on high-surface-area carbon and electrochemically tested, showing a 6-fold higher mass activity and 10-fold higher specific activity toward ethanol oxidation reaction than commercially available Pt catalysts.
基于铂的纳米框架是直接乙醇燃料电池中乙醇氧化反应最有前景的催化剂之一。了解制备这些基于中空纳米框架的催化剂的机制很重要。在此，首次用小的SnO纳米颗粒修饰了具有铂表皮的PtRhNi菱形十二面体纳米框架，并将其用作乙醇氧化反应的高效催化剂。此外，通过结合合成各阶段的非原位扫描透射电子显微镜和能量色散X射线光谱观察结果，以及密度泛函理论计算，有可能追踪作为PtRhNi纳米框架前体的实心菱形十二面体PtRhNi纳米颗粒的合成路线。从实心PtRhNi纳米颗粒的镍核进行化学蚀刻后，所得纳米框架用SnO纳米颗粒修饰。将所得的SnO@PtRhNi异质聚集体沉积在高比表面积碳上并进行电化学测试，结果表明，与市售铂催化剂相比，其对乙醇氧化反应的质量活性高6倍，比活性高10倍。
