Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 17, Pages 6482-6490Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c00384
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Funding
- MOST [2016YFA0203302]
- NSFC [21634003, 51573027, 21875042, 21805044, 21771170]
- STCSM [16JC1400702, 18QA140080, 19QA140080]
- SHMEC [2017-01-07-00-07-E00062]
- Yanchang Petroleum Group
- Program for Eastern Scholars at Shanghai Institutions
- Ontario Research Fund - Research Excellence Program
- NSERC
- Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub through the Office of Science of the U.S. Department of Energy [DE-SC0004993]
- NSF [CBET-1805022]
- DOE AMO
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Ternary oxide electrocatalysts consisting of Sr, Ru, and Ir have been developed to achieve high OER activity and stability in acidic electrolytes. The interaction in the Ru-O-Ir local structure suppresses the participation of lattice oxygen during OER, thus improving stability, while modulation of the electronic structure of active Ru sites optimizes the binding energetics of OER oxo-intermediates.
In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr-Ru-Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm(-2) and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and O-18 isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru-O-Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.
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