Leaky graphene oxide with high quantum yield and dual-wavelength photoluminescence

Leaky graphene oxide with high quantum yield and dual-wavelength photoluminescence
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具有高量子产率和双波长光致发光的泄漏氧化石墨烯

DOI:
10.1016/j.carbon.2016.07.046
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发表时间:
2016-11
期刊:
影响因子:
10.9
通讯作者:
er V. Okotrub
er V. Okotrub
中科院分区:
材料科学2区
文献类型:
--
作者:
Igor P. Asanov;Lyubov G. Bulusheva;Huaihe Song;Alex;er V. Okotrub

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采用混酸氧化氧化石墨烯的方法制备了克级泄漏氧化石墨烯。LGO表现出双波长光致发光,其绝对量子产率为11.6%。采用水热法、联氨辅助水热法和联氨回流三种途径来降低LGO。含氧官能团和含氮官能团的含量因还原方法的不同而不同。还原的LGO表现出双波长发光蓝移和量子产率的强烈下降。为了了解不同官能团对发光的贡献,根据我们的实验结果,我们用密度泛函理论计算了不同官能团修饰的石墨烯碎片的基态。随着官能团的去除,能隙变宽,表明还原后的荧光发生蓝移。我们认为LGO的蓝绿色荧光是通过量子尺寸效应从小的芳香族结构域中产生的。芳香族结构域周围的官能团导致荧光红移。高的量子产额可能归因于LGO的缺陷和空穴结构。我们的工作为制备高性能的石墨烯基光致发光材料提供了一种简单的方法,并有助于理解双波长发光的本质。
Leaky graphene oxide (LGO) was gram-scale prepared by oxidation of graphite oxide using mixed acid. The LGO showed a dual-wavelength photoluminescence (PL) with the absolute quantum yield of 11.6%. Three routes including hydrothermal method, hydrazine-assisted hydrothermal method, and hydrazine reflux were used to reduce the LGO. The contents of oxygen- and nitrogen-bearing functional groups varied depending on the reduction methods. The reduced LGOs showed a blue-shifted dual-wavelength PL and strong decrease of the quantum yields. To understand the contribution of different kind of functional groups to the PL, we used density functional theory calculation of the ground states of graphene fragments modified by various functional groups according to our experimental results. The energy gaps broadened with the removal of functional groups, indicating the blue-shift of the PL after reduction. We proposed that the blue-green PL of the LGO arose from small aromatic domains by quantum size effect. Functional groups surrounded the aromatic domains induced the red shift of the PL. The high quantum yield may ascribe to the defective and holey structure of the LGO. Our work provided a simple method to prepare high performance graphene based PL materials, and could help for understanding the nature of dual-wavelength PL.
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