期刊
ACS NANO
卷 6, 期 11, 页码 9541-9550出版社
AMER CHEMICAL SOC
DOI: 10.1021/nn302674k
关键词
graphene oxide; nitrogen-doped graphene; iron coordination; oxygen reduction reaction; stability
类别
资金
- Max Planck Society through the program ENERCHEM
- DFG [SPP 1459]
- BMBF LiBZ Project
- BMBF Graphenoid Project
- ESF Project GOSPEL [09-EuroGRAPHENE-FP-001]
- EU Project GENIUS
- ERC grant on NANOGRAPH
The high cost of platinum-based electrocatalysts for the oxygen reduction reaction (ORR) has hindered the practical application of fuel cells. Thanks to its unique chemical and structural properties, nitrogen-doped graphene (NG) is among the most promising metal-free catalysts for replacing platinum. In this work, we have developed a cost-effective synthesis of NG by using cyanamide as a nitrogen source and graphene oxide as a precursor, which led to high and controllable nitrogen contents (4.0% to 12.0%) after pyrolysis. NG thermally treated at 900 degrees C shows a stable methanol crossover effect, high current density (6.67 mA cm(-2)), and durability (similar to 87% after 10 000 cycles) when catalyzing ORR in alkaline solution : Further, iron (Fe) nanoparticles could be incorporated Into NG with the aid of Fe(III) chloride in the synthetic process. This allows one to examine the Influence of non noble metals on the. electrocatalytic performance. Remarkably, we found that NG supported with 5 wt %Fe nanoparticles displayed an excellent methanol crossover effect and high current density (8.20 mA cm(-2)) in an alkaline solution. Moreover, Fe-incorporated NG showed almost four electron transfer processes and superior stability in both alkaline (similar to 94%) and acidic (similar to 85%) solutions, which outperformed the platinum and NG-based catalysts.
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