Journal
NANO ENERGY
Volume 41, Issue -, Pages 417-425Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.nanoen.2017.09.055
Keywords
Electrocatalyst; Coordinatively unsaturated metal sites; ZIF-67; Oxygen evolution reaction
Categories
Funding
- National Natural Science Foundation of China [51402100, 21573066]
- Provincial Natural Science Foundation of Hunan [2016JJ1006, 2016TP1009]
- National Science Foundation [1561886, 1363123]
- US Air Forces MURI program [FA9550-12-1-0037]
- Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education
- Guangdong Province
- Shenzhen Science and Technology Program [JCYJ20170306141659388]
- Directorate For Engineering
- Div Of Civil, Mechanical, & Manufact Inn [1363123] Funding Source: National Science Foundation
- Div Of Civil, Mechanical, & Manufact Inn
- Directorate For Engineering [1561886] Funding Source: National Science Foundation
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Metal-organic-frameworks (MOFs), in which metal ions are single-atomically dispersed, are regarded as one of the most promising single-atom doped catalysts. Co-based species have been considered as a potential candidate to replace the precious RuO2 to electrocatalyze oxygen evolution reaction (OER). Zeolitic imidazolate frameworks-67 (ZIF-67), a Co-containing MOF, may be an excellent precursor for single-atom OER electrocatalysts due to its rich and uniform distribution of cobalt species. In principle, Co ions are fully coordinated (except for those on the surfaces) in ZIF-67 without accessible sites for electrocatalysis. One way to utilize this single-atom material as electrocatalysts is to remove some of the ligands attached to Co atoms to create coordinately unsaturated metal sites (CUMSs) as the catalytic centers for OER. Herein, we, for the first time, have created CUMSs in ZIF-67 through dielectric barrier discharge (DBD) plasma etching. The CUMSs act as excellent catalytic centers for OER with a promising electrocatalytic activity, even comparable to the precious RuO2. Interestingly, the OER activity of the CUMSs is reversible by supplementing the missing ligands. Our density-functional theory calculations also demonstrated the contribution of the unsaturated metal sites to the high catalytic activity for OER.
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