A density functional study on the oxygen reduction reaction mechanism on FeN2-doped graphene
A density functional study on the oxygen reduction reaction mechanism on FeN2-doped graphene
复制标题
FeN2掺杂石墨烯氧还原反应机理的密度泛函研究
DOI：
10.1039/c8nj00995c
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发表时间：
2018-04
期刊：
影响因子：
--
通讯作者：
Ying Wang
中科院分区：
文献类型：
--
作者：
Yuewen Yang;Kai Li;Yanan Meng;Ying Wang;Ying Wang
合理设计杂原子掺杂石墨烯作为高活性、非贵金属的氧还原反应（ORR）电催化剂对燃料电池的商业应用具有重要意义。本文采用密度泛函理论研究了氮化铁掺杂石墨烯（FeN 2-Gra）表面的有机还原催化活性和反应机理。结果表明，与FeN_3-Gra和FeN_4-Gra类似，在FeN_2-Gra上的ORR是一个四电子过程.但FeN_2-Gra与FeN_3-Gra和FeN_4-Gra的反应机理不同。对于FeN 2-Gra，OOH氢化形成OH + OH是动力学上最有利的途径，其中O2氢化形成OOH是具有0.47 eV的能垒的速率决定步骤。该能垒对于FeN 4-Gra小于0.56eV，并且对于FeN 3-Gra远小于0.87eV，对于纯Pt远小于0.86eV。预测工作电位为0.18V。与纯Pt相比，FeN 2-Gra还具有更好的抗CO中毒能力。因此，FeN 2-Gra是良好的ORR催化剂。
The rational design of heteroatom doped graphene as a highly active and non-noble oxygen reduction reaction (ORR) electrocatalyst is significant for the commercial applications of the fuel cells. In this work, the catalytic activity for the ORR and the reaction mechanism on the surface of FeN2 doped graphene (FeN2-Gra) have been studied by using density functional theory. The results indicate that the ORR is a four-electron process on FeN2-Gra, similar to FeN3-Gra and FeN4-Gra. But FeN2-Gra shows quite different reaction mechanisms compared with FeN3-Gra and FeN4-Gra. For FeN2-Gra, the OOH hydrogenation to form OH + OH is the kinetically most favorable pathway, in which the O2 hydrogenation to form OOH is the rate-determining step with an energy barrier of 0.47 eV. This energy barrier is smaller than 0.56 eV for FeN4-Gra, and much smaller than 0.87 eV for FeN3-Gra and 0.86 eV for pure Pt. The predicted working potential is 0.18 V. FeN2-Gra also has better capability of resisting CO poisoning compared with pure Pt. Consequently, the FeN2-Gra is a good ORR catalyst.
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用于 OER 和 ORR 的双功能 CoNx 嵌入石墨烯电催化剂：理论评估
影响因子：
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作者：
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影响因子：
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作者：
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作者：
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通讯作者：
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作者：
Koslowski, Ulrike I.;Abs-Wurmbach, Irmgard;Bogdanoff, Peter
通讯作者：
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DOI：
10.1039/c5cp01530h
发表时间：
2015-05
期刊：
Physical chemistry chemical physics : PCCP
影响因子：
--
作者：
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通讯作者：
D. Song;Baowei Song;Hai-bao Hu;Xiaosong Du;Feng Zhou