School of Computational Sciences, Korea Institute for Advanced Study, Seoul, 130-722, Korea.
Nanoscale. 2012 Jan 21;4(2):417-20. doi: 10.1039/c1nr11307k. Epub 2011 Nov 24.
Based on first principles density functional theory calculations we explored energetics of oxygen reduction reaction over pristine and nitrogen-doped graphene with different amounts of nitrogen doping. The process of oxygen reduction requires one more step than the same reaction catalyzed by metals. Results of calculations evidence that for the case of light doped graphene (about 4% of nitrogen) the energy barrier for each step is lower than for the same process on a Pt surface. In contrast to the catalysis on a metal surface the maximal coverage of doped graphene is lower and depends on the corrugation of graphene. Changes of the energy barriers caused by oxygen load and corrugation are also discussed.
基于第一性原理密度泛函理论计算，我们研究了在原始和不同氮掺杂量的氮掺杂石墨烯上氧还原反应的能量学。氧还原反应的过程比金属催化的相同反应多需要一个步骤。计算结果表明，对于轻掺杂石墨烯（约 4%的氮）的情况，每个步骤的能量势垒都低于在 Pt 表面上的相同过程。与金属表面的催化作用相反，掺杂石墨烯的最大覆盖度较低，并且取决于石墨烯的波纹度。还讨论了氧负载和波纹度引起的能垒变化。
