To develop more ideal bifunctional heteroatom-doped carbon electrocatalysts toward the oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) for regenerative fuel cells and rechargeable metal–air batterie...To develop more ideal bifunctional heteroatom-doped carbon electrocatalysts toward the oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) for regenerative fuel cells and rechargeable metal–air batteries, herein, tobacco-derived N-containing ordered mesoporous carbon(N-OMC) electrocatalysts with different N species distributions are designed. Results indicate that the as-prepared N-OMC with more pyrrolic and pyridinic Ns exhibits much higher activities for the ORR and OER than N-OMC with more graphitic N in both acidic and alkaline media, suggesting that the increase of pyrrolic and pyridinic Ns favors the improvement of ORR and OER activities of the N-containing carbon catalysts, and showing a great potential for the designing of more effective, lower-cost ORR and OER bifunctional electrocatalysts for future regenerative fuel cells and rechargeable metal–air batteries.展开更多
Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of gra...Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of graphitic carbon for the oxygen-reduction reaction (ORR) both in acidic and alkaline media, and the materials exhibited high electrocatalytic activity, long-term stability, and excellent tolerance to crossover effects especially in alkaline media. Quantum mechanics calculations with the density functional theory demonstrated that the changes in charge density and energetic characteristics of frontier orbitals for the P-doped graphene sheet could facilitate the ORR.展开更多
基金financial support from the National Natural Science Foundation of China(No.21376257)the Jiangsu Provincial Natural Science Foundation of China(No.BK20131112)
文摘To develop more ideal bifunctional heteroatom-doped carbon electrocatalysts toward the oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) for regenerative fuel cells and rechargeable metal–air batteries, herein, tobacco-derived N-containing ordered mesoporous carbon(N-OMC) electrocatalysts with different N species distributions are designed. Results indicate that the as-prepared N-OMC with more pyrrolic and pyridinic Ns exhibits much higher activities for the ORR and OER than N-OMC with more graphitic N in both acidic and alkaline media, suggesting that the increase of pyrrolic and pyridinic Ns favors the improvement of ORR and OER activities of the N-containing carbon catalysts, and showing a great potential for the designing of more effective, lower-cost ORR and OER bifunctional electrocatalysts for future regenerative fuel cells and rechargeable metal–air batteries.
基金supported by the Guangdong Provincial Science and Technology Project of China (2011B010400016)China Postdoctoral Science Foundation (No. 20110490878)
文摘Phosphorus-doped carbon nanospheres without any metal residues were synthesized and characterized. The results revealed that the doping phosphorus atoms could significantly improve the electrocatalytic activity of graphitic carbon for the oxygen-reduction reaction (ORR) both in acidic and alkaline media, and the materials exhibited high electrocatalytic activity, long-term stability, and excellent tolerance to crossover effects especially in alkaline media. Quantum mechanics calculations with the density functional theory demonstrated that the changes in charge density and energetic characteristics of frontier orbitals for the P-doped graphene sheet could facilitate the ORR.