期刊
NATURE CHEMISTRY
卷 3, 期 8, 页码 634-641出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1095
关键词
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资金
- National Science Foundation of China [20325620, 20773124]
- Ministry of Science and Technology of China [NKBRSF 2007CB815200, 2011CB932400]
- US Department of Energy, Office of Energy Efficiency and Renewable Energy
Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H-2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.
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