Shuai Zhang, Leilei Yin, Qian Liu, Guangtong Hai, Yaping Du
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引用次数: 0
Abstract
The ligand effect in alloy catalysts is one of the decisive parameters of the catalytic performance. However, the strong interrelation between the ligand effect and the geometric effect of the active atom and its neighbors as well as the systematic alteration of the microenvironment of the active site makes the active mechanism unclear. Herein, Pt3Tm, Pt3Yb, and Pt3Lu with a cubic crystal system (Pm-3m) were selected. With the difference of Pt-Pt interatomic distance within 0.02 Å, we minimize the geometric effect to realize the disentanglement of the system. Through precise characterization, due to the low electronegativity of Ln (Ln = Tm, Yb, and Lu) and the ligand effect in the alloy, the electronic structure of Pt is continuously optimized, which improves the electrochemical methanol oxidation reaction (MOR) performance. The Ln electronegativity has a linear relationship with the MOR performance, and Pt3Yb/C achieves a high mass activity of up to 11.61 A mgPt-1, which is the highest value reported so far in Pt-based electrocatalysts. The results obtained in this study provide fundamental insights into the mechanism of ligand effects on the enhancement of electrochemical activity in rare-earth nanoalloys.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.