First-Principles Study on Nitrobenzene-Doped Graphene as a Metal Free Electrocatalyst for Oxygen Reduction Reaction

被引：45

作者：

Jiao, Menggai ^{[1
,3
]}

Song, Wei ^{[2
]}

Li, Kai ^{[1
]}

Wang, Ying ^{[1
]}

Wu, Zhijian ^{[1
]}

机构：

[1] Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Peoples R China

[2] Xinxiang Univ, Phys & Elect Engn Dept, Xinxiang 453003, Peoples R China

[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2016年 / 120卷 / 16期

基金：

中国国家自然科学基金;

关键词：

DENSITY-FUNCTIONAL-THEORY; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; AUGMENTED-WAVE METHOD; FUEL-CELLS; BASIS-SET; NITROGEN; CATALYSTS; TRANSITION; BORON;

D O I：

10.1021/acs.jpcc.6b02097

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The electrocatalyst, nitrobenzene molecular doped graphene, for the oxygen reduction reaction (ORR) is investigated by the first-principles calculations. We find that zigzag edge (Z), doped armchair edge (NBA), and the opposite-side edge of doped zigzag nanoribbon (NBZ-2) are three active centers that contribute to the efficient catalytic performance. Our calculations suggest that such excellent electrocatalytic properties originate from the induced high asymmetry spin density and charge redistribution. The calculated onsite potentials are -0.13, -0.43, and -0.11 V for Z, NBA, and NBZ-2, which are close to the experimental values of -0.20 V on NBG and -0.24 V on graphene. We also find that the electrocatalytic activity and the tolerance of methanol depend on the doped configurations. Therefore, the carefully controllable synthesis is highly expected to further improve the ORR activity of nitrobenzene-doped graphene.

引用

页码：8804 / 8812

页数：9

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