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Temperature-driven phase transformation and element segregation in pd-ru immiscible alloy nanoparticles:Spatial resolving of elements and insights for electrocatalysis

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Nano Research 2023年第7期16卷 9968-9976页

作者： Hui Li Zheng Hu Yu Zhang Wenbo Zhao Yuyao Zeng Wei Zhou Shi Hu Department of Chemistry School of ScienceTianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300072China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China Department of Physics School of ScienceTianjin Key Laboratory of Molecular Optoelectronic ScienceTianjin UniversityTianjin 300072China

Bimetallic alloys could form three typical structures including solid solution,heterostructure,and intermetallic compound,depending on the interactions between identical and different *** the trend can be predicted by the types of binary phase diagram,different synthetic protocols will trap the system in various kinetic intermediates among the three typical ***,we studied the phase evolution and elemental segregation in the alloy nanoparticles of immiscible pd-ru before and after thermal *** developing an analysis method of local element segregation(LES)based on the energy dispersive spectroscopy(EDS)mapping signals,we were able to quantify the mixing of pd and ru atoms during the gradual phase transition from face-centered cubic(fcc)to hexagonal close packed(hcp).Density functional theory was also applied to calculate the energies of all possible pdru4 structures(93 fcc models and 267 hcp models),which helps to rationalize the phase transition and element *** annealing process also leads to the change of the electronic structure,which further influences the performance in the electrocatalytic hydrogen evolution *** highest activity of pdru4-400 was largely attributed to the proper interface between the pd-rich fcc phase and ru-rich hcp phase,as revolved by the above methods.

关键词： pd-ru alloy short-range order local element segregation hydrogen evolution reaction

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