Boosting Activation of Oxygen Molecules on C60 Fullerene by Boron Doping
Boosting Activation of Oxygen Molecules on C60 Fullerene by Boron Doping
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DOI：
10.1002/cphc.201402620
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发表时间：
2015-02-02
期刊：
影响因子：
2.9
通讯作者：
Zhao, Xiang
中科院分区：
文献类型：
--
作者：
Li, Qiao-Zhi;Zheng, Jia-Jia;Zhao, Xiang
采用杂化密度泛函方法系统研究了氧分子在硼掺杂C-60富勒烯（C59 B）表面的活化及随后的水生成反应.结果表明，C59 B显示出良好的能力，激活氧分子的动力学和热力学。氧分子首先被吸附在硼原子上，由于其高的正电荷和自旋密度，硼原子被确定为C59 B中对O-2吸附最具反应性的位点。吸附结构C59 BO 2可以进一步异构化形成两种反应势垒小的产物。这两种结构上的水形成反应是积极有利的，并建议由C59 B催化的氧还原反应的四电子机制。本工作为硼掺杂富勒烯的催化性能提供了可靠的理论依据，有助于富勒烯催化剂的研究。
The activation of oxygen molecules on boron-doped C-60 fullerene (C59B) and the subsequent water formation reaction are systematically investigated by using hybrid density functional calculations. Results indicate that C59B shows a favorable ability to activate oxygen molecules both kinetically and thermodynamically. The oxygen molecule is first adsorbed on the boron atom, which is identified to be the most reactive site in C59B for O-2 adsorption because of its high positive charge and spin density. The adsorption structure C59BO2 can further isomerize to form two products with small reaction barriers. Water formation reactions upon these two structures are energetically favorable and suggest a four-electron mechanism for the oxygen reduction reaction catalyzed by C59B. This work provides a reliable theoretical insight into the catalytic properties of boron-doped fullerene, which is believed to be helpful to explore fullerene catalysts.