期刊
CHEMCATCHEM
卷 11, 期 24, 页码 6039-6050出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201900887
关键词
Cobalt-based catalyst; N, S co-doped; Co9S8; carbon nanotubes; oxygen reduction reaction
资金
- NSFC [21573286, 21173269, 91127040, 21576288, U1662104]
- Ministry of Science and Technology of China [2011BAK15B05]
- Specialized Research Fund for the Doctoral Program of Higher Education [20130007110003]
- Science Foundation of China University of Petroleum, Beijing [2462015YQ0304]
- open fund of the State Key Laboratory of Chemical Resource Engineering, Beijing
Herein, a novel electrocatalysts of cobalt nanoparticles embedded in N, S co-doped carbon matrix derived by in situ reducing Co9S8 are designed and prepared successfully through two-calcination methods, and applied for oxygen reduction reaction (ORR). Due to the large surface area and pore volume, richness of defects existing the carbon nanotubes, interaction of S species and N species and special direction of electron transfers between Co and S ions, the earth-abundant and low-cost CoSMe-0.5-800 presents a highly efficient ORR activity and stability. The onset potential, half-wave potential and limiting current density of CoSMe-0.5-800 are 0.95 V, 0.85 V, and 4.31 mA cm(-2), which are higher than that of commercial Pt/C (0.93 V, 0.83 V, 4.19 mA cm(-2)). More importantly, the interaction between N and S heteroatoms in system gets revealed, that S resources can help to improve the degree of N doping and raise the ratio of pyridinic N species working as the active site for ORR. With the increase of S resources, electrons that should have been transferred from cobalt to sulfur have moved in the opposite direction, which has a negative effect on ORR active performance. This work shows the potential to design advanced Co-based N, S co-doped catalysts with high electrochemical performance and low cost, which could be applied for fuel cells and other devices.
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