Engineering electrocatalytic activity in nanosized perovskite cobaltite through surface spin-state transition

Shiming Zhou (), Xianbing Miao, Xu Zhao, Chao Ma, Yuhao Qiu, Zhenpeng Hu (), Jiyin Zhao, Lei Shi and Jie Zeng ()
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Shiming Zhou: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Xianbing Miao: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Xu Zhao: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Chao Ma: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Yuhao Qiu: School of Physics, Nankai University
Zhenpeng Hu: School of Physics, Nankai University
Jiyin Zhao: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Lei Shi: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China
Jie Zeng: Hefei National Laboratory for Physics Sciences at the Microscale, Hefei Science Center, University of Science and Technology of China

Nature Communications, 2016, vol. 7, issue 1, 1-7

Abstract: Abstract The activity of electrocatalysts exhibits a strongly dependence on their electronic structures. Specifically, for perovskite oxides, Shao-Horn and co-workers have reported a correlation between the oxygen evolution reaction activity and the eg orbital occupation of transition-metal ions, which provides guidelines for the design of highly active catalysts. Here we demonstrate a facile method to engineer the eg filling of perovskite cobaltite LaCoO3 for improving the oxygen evolution reaction activity. By reducing the particle size to ∼80 nm, the eg filling of cobalt ions is successfully increased from unity to near the optimal configuration of 1.2 expected by Shao-Horn’s principle. Consequently, the activity is significantly enhanced, comparable to those of recently reported cobalt oxides with eg∼1.2 configurations. This enhancement is ascribed to the emergence of spin-state transition from low-spin to high-spin states for cobalt ions at the surface of the nanoparticles, leading to more active sites with increased reactivity.

Date: 2016
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DOI: 10.1038/ncomms11510

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