Citation: WANG Jun, LI Li, WEI Zi-Dong. Density Functional Theory Study of Oxygen Reduction Reaction on Different Types of N-Doped Graphene[J]. Acta Physico-Chimica Sinica, ;2016, 32(1): 321-328. doi: 10.3866/PKU.WHXB201512091 shu

Density Functional Theory Study of Oxygen Reduction Reaction on Different Types of N-Doped Graphene

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State Key Laboratory of Power Transmission Equipment & System Security and New Technology; College of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, P. R. China

Corresponding author: LI Li, WEI Zi-Dong,
Received Date: 20 October 2015
Available Online: 9 December 2015
Fund Project: 国家自然科学基金(21176271,21376284)资助项目 (21176271,21376284)

N-doped graphene has aroused much interest owing to its high activity and stability in oxygen reduction reaction (ORR) catalysis. However, the contribution of different types of N-doped graphene to ORR activity remains in dispute. Based on this issue, this paper conducts a comparative study of the ORR on graphitic N-doped graphene (GNG) and pyridinic N-doped grapheme (PNG). Band structure calculations show that the conductivity of GNG decreases as the nitrogen content increases; while that of PNG first increases to the highest at nitrogen content of 4.2% (atomic fraction), and then decreases. The conductivity of PNG is always higher than GNG when the doped nitrogen content is greater than 1.4%. Additionally, the free energy diagram of ORR shows that protonation of O₂ is the potential-determining step among the whole ORR process, and the free energy change of this step on GNG is lower than on PNG, suggesting that GNG has higher ORR activity than PNG if their electron transport ability are the same. When the N content is lower than 2.8%, the conductivity difference between GNG and PNG is almost negligible, thus GNG with a higher capacity of O₂ protonation exhibits better ORR activity than PNG. When the N content is greater than 2.8%, in this case, conductivity rather than free energy change will dominate, therefore the ORR on PNG will occur faster than on GNG because of its higher conductivity.
- Oxygen reduction reaction,
- Nitrogen doped graphene,
- Pyridinic nitrogen,
- Graphitic nitrogen,
- Density functional theory
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