Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction

• Published in: Science (American Association for the Advancement of Science) 2009-02, Vol.323 (5915), p.760-764
• Main Authors: Gong, Kuanping, Du, Feng, Xia, Zhenhai, Durstock, Michael, Dai, Liming
• Format: Article
• Language: English
• Subjects: Applied sciences; Atoms; Carbon nanotubes; Catalysts; Chemical engineering; Electrodes; Energy; Energy. Thermal use of fuels; Equipments for energy generation and conversion: thermal, electrical, mechanical energy, etc; Exact sciences and technology; Fuel cells; Materials science; Molecules; Nanotubes; Nitrogen; Oxidation; Oxygen; Steady state current
• ISSN: 0036-8075; 1095-9203
• DOI: 10.1126/science.1168049

The large-scale practical application of fuel cells will be difficult to realize if the expensive platinum-based electrocatalysts for oxygen reduction reactions (ORRs) cannot be replaced by other efficient, low-cost, and stable electrodes. Here, we report that vertically aligned nitrogen-containing carbon nanotubes (VA-NCNTs) can act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction in alkaline fuel cells. In air-saturated 0.1 molar potassium hydroxide, we observed a steady-state output potential of -80 millivolts and a current density of 4.1 milliamps per square centimeter at -0.22 volts, compared with -85 millivolts and 1.1 milliamps per square centimeter at -0.20 volts for a platinum-carbon electrode. The incorporation of electron-accepting nitrogen atoms in the conjugated nanotube carbon plane appears to impart a relatively high positive charge density on adjacent carbon atoms. This effect, coupled with aligning the NCNTs, provides a four-electron pathway for the ORR on VA-NCNTs with a superb performance.