Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution

Jie Dai, Yinlong Zhu (), Hassan A. Tahini, Qian Lin, Yu Chen, Daqin Guan, Chuan Zhou, Zhiwei Hu, Hong-Ji Lin, Ting-Shan Chan, Chien-Te Chen, Sean C. Smith, Huanting Wang, Wei Zhou and Zongping Shao ()
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Jie Dai: Nanjing Tech University
Yinlong Zhu: Monash University
Hassan A. Tahini: Australian National University
Qian Lin: Monash University
Yu Chen: Monash University
Daqin Guan: Nanjing Tech University
Chuan Zhou: Nanjing Tech University
Zhiwei Hu: Max Planck Institute for Chemical Physics of Solids
Hong-Ji Lin: National Synchrotron Radiation Research Center
Ting-Shan Chan: National Synchrotron Radiation Research Center
Chien-Te Chen: National Synchrotron Radiation Research Center
Sean C. Smith: Australian National University
Huanting Wang: Monash University
Wei Zhou: Nanjing Tech University
Zongping Shao: Nanjing Tech University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract The state-of-the-art active HER catalysts in acid media (e.g., Pt) generally lose considerable catalytic performance in alkaline media mainly due to the additional water dissociation step. To address this issue, synergistic hybrid catalysts are always designed by coupling them with metal (hydro)oxides. However, such hybrid systems usually suffer from long reaction path, high cost and complex preparation methods. Here, we discover a single-phase HER catalyst, SrTi0.7Ru0.3O3-δ (STRO) perovskite oxide highlighted with an unusual super-exchange effect, which exhibits excellent HER performance in alkaline media via atomic-scale synergistic active centers. With insights from first-principles calculations, the intrinsically synergistic interplays between multiple active centers in STRO are uncovered to accurately catalyze different elementary steps of alkaline HER; namely, the Ti sites facilitates nearly-barrierless water dissociation, Ru sites function favorably for OH* desorption, and non-metal oxygen sites (i.e., oxygen vacancies/lattice oxygen) promotes optimal H* adsorption and H2 desorption.

Date: 2020
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DOI: 10.1038/s41467-020-19433-1

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