Geometric and electronic properties of graphene modified by "external" N-containing groups.
Geometric and electronic properties of graphene modified by "external" N-containing groups.
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DOI：
10.1039/c4cp03069a
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发表时间：
2014-09
期刊：
影响因子：
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通讯作者：
Xinde Wang;Q. Cai;G. Zhuang;Xing Zhong;Donghai Mei;Xiaonian Li;Jianguo Wang
中科院分区：
文献类型：
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作者：
Xinde Wang;Q. Cai;G. Zhuang;Xing Zhong;Donghai Mei;Xiaonian Li;Jianguo Wang
采用第一性原理自旋极化密度泛函理论（DFT）计算，研究了“外部”含氮基团（吡啶衍生物）通过单键或双键方式修饰石墨烯的结构和电子性质.我们的研究结果表明，在最稳定的结构中，吡啶衍生物和石墨烯之间的键合涉及吡啶衍生物的邻位碳，正如Bader电荷分析所证实的。通过[2+2]环加成，例如，双键模式（DBPyNG）是由吡啶衍生物的前线轨道与石墨烯的前线轨道之间的匹配引起的，这导致形成更强的化学键。有趣的是，SBPyNG的电子结构态密度（DOS）分析显示，自旋向上和自旋向下部分明显分裂，而双键吡啶衍生物修饰的石墨烯（DBPyNG）则不是这种情况。
Using first-principles spin polarized density functional theory (DFT) calculations, we investigated structures and electronic properties of "external" nitrogen-containing group (pyridine derivatives) modified graphene via a single or a double bonding mode. Our results show that in the most stable structures, the bonding between pyridine derivatives and graphene involves the ortho-carbon of pyridine derivatives, as confirmed by the Bader charge analysis. The enhanced stability of pyridine derivatives on graphene by [2+2] cycloaddition, e.g., a double bonding mode (DBPyNG), is caused by the matches between frontier orbitals of pyridine derivatives and those of graphene, which leads to the formation of stronger chemical bonds. Interestingly, electronic structure density of states (DOS) analysis of SBPyNG reveals that the spin-up and spin-down parts are clearly split while it is not the case for the double bonding pyridine derivative modified graphene (DBPyNG).