Energetics of Nanoparticle Exsolution from Perovskite Oxides

Gao, Yang1,2; Lu, Ziheng1; You, Tsam Lung1; Wang, Jian1; Xie, Lin3; He, Jiaqing3; Ciucci, Francesco1,4

2018-07-05

10.1021/acs.jpclett.8b01380

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

The presence of active metal nanoparticles on the surface significantly increases the electrochemical performance of ABO(3) perovskite oxide materials. While conventional deposition methods can improve the activity, in situ exsolution produces nanoparticles with far greater stability. The migration of transition metal atoms toward the surface is expected to affect the exsolution process. To study the energetics, we use ab initio computations combined with experiments in a SrTiO3-based model system. Our calculations show that Ni preferentially segregates toward the (100)-oriented and SrTiO-terminated surfaces, note that this orientation is identical to one reported by the Irvine and Gorte groups. Vacancies in the Sr-site and O-site promote the segregation of Ni, while placing La on the Sr-site has an opposite effect. The corresponding experiments are in agreement with the computational predictions. Fast nanoparticle growth and activity enhancement are found in STO system with Sr vacancies and without La. The approach developed in this Letter could be used to study the mechanism of exsolution in other material systems, and possibly lead to the development of new compositions capable of nanoparticle exsolution with higher activity and stability.

SCI ; EI

英语

NI期刊

其他

Science, Technology, and Innovation Commission of Shenzhen Municipality[JCYJ20150831142508365] ; Science, Technology, and Innovation Commission of Shenzhen Municipality[KQTD2016 022619565991]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000438314800035

AMER CHEMICAL SOC

20182605357215

Calculations ; Perovskite ; Strontium titanates ; Transition metals

Minerals:482.2 ; Metallurgy and Metallography:531 ; Nanotechnology:761 ; Chemical Products Generally:804 ; Mathematics:921

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Mech & Aerosp Engn, Hong Kong, Hong Kong, Peoples R China
2.Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
4.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Hong Kong, Hong Kong, Peoples R China

Gao, Yang,Lu, Ziheng,You, Tsam Lung,et al. Energetics of Nanoparticle Exsolution from Perovskite Oxides[J]. Journal of Physical Chemistry Letters,2018,9(13):3772-3778.

Gao, Yang.,Lu, Ziheng.,You, Tsam Lung.,Wang, Jian.,Xie, Lin.,...&Ciucci, Francesco.(2018).Energetics of Nanoparticle Exsolution from Perovskite Oxides.Journal of Physical Chemistry Letters,9(13),3772-3778.

Gao, Yang,et al."Energetics of Nanoparticle Exsolution from Perovskite Oxides".Journal of Physical Chemistry Letters 9.13(2018):3772-3778.