Key Laboratory for Design and Synthesis of Functionalized Materials and Green Catalysis, School of Chemistry and Chemical Engineering, Harbin Normal University, Harbin, People's Republic of China.
J Mol Model. 2012 May;18(5):2043-54. doi: 10.1007/s00894-011-1226-x. Epub 2011 Sep 1.
Exploring and evaluating the potential applications of two-dimensional graphene is an increasingly hot topic in graphene research. In this paper, by studying the adsorption of NO, N(2)O, and NO(2) on pristine and silicon (Si)-doped graphene with density functional theory methods, we evaluated the possibility of using Si-doped graphene as a candidate to detect or reduce harmful nitrogen oxides. The results indicate that, while adsorption of the three molecules on pristine graphene is very weak, Si-doping enhances the interaction of these molecules with graphene sheet in various ways: (1) two NO molecules can be adsorbed on Si-doped graphene in a paired arrangement, while up to four NO(2) molecules attach to the doped graphene with an average adsorption energy of -0.329 eV; (2) the N(2)O molecule can be reduced easily to the N(2) molecule, leaving an O-atom on the Si-doped graphene. Moreover, we find that adsorption of NO and NO(2) leads to large changes in the electronic properties of Si-doped graphene. On the basis of these results, Si-doped graphene can be expected to be a good sensor for NO and NO(2) detection, as well as a metal-free catalyst for N(2)O reduction.
探索和评估二维石墨烯的潜在应用是石墨烯研究中一个日益热门的话题。在本文中，我们通过使用密度泛函理论方法研究了一氧化氮（NO）、氧化亚氮（N(2)O）和二氧化氮（NO(2)）在原始和硅（Si）掺杂石墨烯上的吸附，评估了 Si 掺杂石墨烯作为候选材料用于检测或减少有害氮氧化物的可能性。结果表明，虽然这三种分子在原始石墨烯上的吸附非常弱，但 Si 掺杂以各种方式增强了这些分子与石墨烯片之间的相互作用：（1）两个 NO 分子可以在 Si 掺杂的石墨烯上以配对的方式吸附，而多达四个 NO(2)分子以平均吸附能为-0.329eV 的形式附着在掺杂的石墨烯上；（2）N(2)O 分子很容易被还原为 N(2)分子，在 Si 掺杂的石墨烯上留下一个 O 原子。此外，我们发现 NO 和 NO(2)的吸附导致 Si 掺杂石墨烯的电子性质发生了很大的变化。基于这些结果，可以预期 Si 掺杂石墨烯将成为一种用于检测 NO 和 NO(2)的良好传感器，以及一种用于还原 N(2)O 的无金属催化剂。
