期刊
ENERGY STORAGE MATERIALS
卷 13, 期 -, 页码 142-150出版社
ELSEVIER
DOI: 10.1016/j.ensm.2018.01.008
关键词
CO2 activation; Hierarchical structures; Metal-nitrogen-carbon catalysts; Electrocatalysis; Oxygen reduction
资金
- National Key Research and Development Program of China [2016YFB0700204]
- NSFC [51602332, 51502327]
- Science and Technology Commission of Shanghai Municipality [15520720400, 15YF1413800, 14DZ2261203, 16DZ2260603]
- One Hundred Talent Plan of Chinese Academy of Sciences
- National Thousand Youth Talents program of China
- Ningbo program [3315]
Iron-nitrogen-doped carbon materials (Fe-N-C) have emerged as the most promising nonprecious alternative catalysts for commercial Pt/C toward oxygen reduction reaction (ORR). However, the general synthesis of Fe-N-C catalysts involves complex pyrolysis reactions, which not only obtains the difficulty in optimizing pore structures, but also leads to low porosity and specific surface area due to lacking of efficient pore regulation. Herein, we report an efficient post Fe-doping strategy to synthesize high-performance Fe-N-C catalysts using activated N-doped carbon spheres (ANCSs) with improved porosity as the supports. Large amount of micropores in the ANCSs generated by CO2 activation are advantageous for enhanced exposure of N-functional groups which can efficiently complex more Fe ions during post Fe-doping, enabling the facile formation and increasing the accessibility of high-density of Fe-N-x active sites onto the pore surfaces. The resulting Fe-N-C catalysts demonstrated well-defined hierarchical micro-/mesoporosity, large surface area and optimized active sites. Ascribed to the synergy of the above factors, they showed very high ORR activity with a four-electron dominant pathway superior and comparable to that of 20 wt% Pt/C in alkaline and acidic electrolyte, respectively, also presenting excellent stability and methanol tolerance. The present research paves a new avenue for preparing various metal-N-C catalysts used in heterogeneous catalysis, batteries and super-capacitors.
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