Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 12, Pages 13878-13887Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b22577
Keywords
non-precious-metal catalyst; single/paired atoms; metal-organic framework (MOF); oxygen reduction reaction (ORR); 2D materials
Funding
- National Natural Science Foundation of China (NSFC) [21776104, 21476088]
- National Key Research and Development Program of China [2016YFB0101201, 2017YFB0102900]
- Guangdong Provincial Department of Science and Technology [2015B010106012]
- Guangzhou Science, Technology and Innovation Committee [2016GJ006, 201504281614372]
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Developing efficient non-precious-metal catalysts to accelerate the sluggish oxygen reduction reaction (ORR) is highly desired but remains a great challenge. Herein, using 2D bimetallic Zn/Fe-MOF as the precursor and g-C(3)N(4 )as the nitrogen source and stabilizer, porous carbon nanosheets doped with large amounts of single/paired Fe atoms (3.89 wt %) and N (10.28 wt %) are successfully prepared. It is found that the addition of g-C3N4 plays a key role in achieving a high loading of Fe single/paired atoms, and the 2D nanosheet structure gives the materials a high surface area and highly porous structure, resulting in outstanding ORR catalytic activity in both alkaline and acidic solutions. Our optimal sample achieved half-wave potentials in alkaline and acid media of up to 0.86 and 0.79 V (vs reversible hydrogen electrode (RHE)), respectively, values 20 mV higher than a commercial Pt/C catalyst in an alkaline medium and only 60 mV lower than Pt/C in an acidic medium. Moreover, its ORR durability was superior to that of commercial Pt/C in both electrolytes. We found that almost all the doped Fe in the sample existed as single or paired atoms coordinated with N. This work may provide an effective strategy for preparing high-performance catalysts bearing single/paired atoms by using MOFs as precursors.
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