Abstract
The oxygen reduction reaction (ORR) - one of the two half-reactions in fuel cells - is one of the bottlenecks that has prevented fuel cells from finding a wide range of applications today. This is because ORR is inherently a sluggish reaction; it is also because inexpensive and sustainable ORR electrocatalysts that are not only efficient but also are based on earth-abundant elements are hard to come by. Herein we report the synthesis of novel carbon-based materials that can contribute to solving these challenges associated with ORR. Mesoporous oxygen- and nitrogen-doped carbons were synthesized from in situ polymerized mesoporous silica-supported polyaniline (PANI) by carbonization of the latter, followed by etching away the mesoporous silica template from it. The synthetic method also allowed the immobilization of different metals such as Fe and Co easily into the system. While all the resulting materials showed outstanding electrocatalytic activity toward ORR, the metal-free, PANI-derived mesoporous carbon (dubbed PDMC), in particular, exhibited the highest activity, challenging conventional paradigms. This unprecedented activity by the metal-free PDMC toward ORR was attributed to the synergetic activities of nitrogen and oxygen (or hydroxyl) species that were implanted in it by PANI/mesoporous silica during pyrolysis.
| Original language | English |
|---|---|
| Pages (from-to) | 7823-7826 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 135 |
| Issue number | 21 |
| DOIs | |
| Publication status | Published - May 29 2013 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Efficient metal-free electrocatalysts for oxygen reduction : Polyaniline-derived N- and O-doped mesoporous carbons. / Silva, Rafael; Voiry, Damien; Chhowalla, Manish; Asefa, Teddy.
In: Journal of the American Chemical Society, Vol. 135, No. 21, 29.05.2013, p. 7823-7826.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Efficient metal-free electrocatalysts for oxygen reduction
T2 - Polyaniline-derived N- and O-doped mesoporous carbons
AU - Silva, Rafael
AU - Voiry, Damien
AU - Chhowalla, Manish
AU - Asefa, Teddy
PY - 2013/5/29
Y1 - 2013/5/29
N2 - The oxygen reduction reaction (ORR) - one of the two half-reactions in fuel cells - is one of the bottlenecks that has prevented fuel cells from finding a wide range of applications today. This is because ORR is inherently a sluggish reaction; it is also because inexpensive and sustainable ORR electrocatalysts that are not only efficient but also are based on earth-abundant elements are hard to come by. Herein we report the synthesis of novel carbon-based materials that can contribute to solving these challenges associated with ORR. Mesoporous oxygen- and nitrogen-doped carbons were synthesized from in situ polymerized mesoporous silica-supported polyaniline (PANI) by carbonization of the latter, followed by etching away the mesoporous silica template from it. The synthetic method also allowed the immobilization of different metals such as Fe and Co easily into the system. While all the resulting materials showed outstanding electrocatalytic activity toward ORR, the metal-free, PANI-derived mesoporous carbon (dubbed PDMC), in particular, exhibited the highest activity, challenging conventional paradigms. This unprecedented activity by the metal-free PDMC toward ORR was attributed to the synergetic activities of nitrogen and oxygen (or hydroxyl) species that were implanted in it by PANI/mesoporous silica during pyrolysis.
AB - The oxygen reduction reaction (ORR) - one of the two half-reactions in fuel cells - is one of the bottlenecks that has prevented fuel cells from finding a wide range of applications today. This is because ORR is inherently a sluggish reaction; it is also because inexpensive and sustainable ORR electrocatalysts that are not only efficient but also are based on earth-abundant elements are hard to come by. Herein we report the synthesis of novel carbon-based materials that can contribute to solving these challenges associated with ORR. Mesoporous oxygen- and nitrogen-doped carbons were synthesized from in situ polymerized mesoporous silica-supported polyaniline (PANI) by carbonization of the latter, followed by etching away the mesoporous silica template from it. The synthetic method also allowed the immobilization of different metals such as Fe and Co easily into the system. While all the resulting materials showed outstanding electrocatalytic activity toward ORR, the metal-free, PANI-derived mesoporous carbon (dubbed PDMC), in particular, exhibited the highest activity, challenging conventional paradigms. This unprecedented activity by the metal-free PDMC toward ORR was attributed to the synergetic activities of nitrogen and oxygen (or hydroxyl) species that were implanted in it by PANI/mesoporous silica during pyrolysis.
UR - http://www.scopus.com/inward/record.url?scp=84878391408&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84878391408&partnerID=8YFLogxK
U2 - 10.1021/ja402450a
DO - 10.1021/ja402450a
M3 - Article
C2 - 23646856
AN - SCOPUS:84878391408
VL - 135
SP - 7823
EP - 7826
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 21
ER -