Multicolor fluorescent emission of graphene oxide and its application in fluorescence imaging
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摘要: 氧化石墨烯作为石墨烯的一种带隙打开的衍生物，极大地丰富了其光学性质，并拓展了它在传感和成像方面的应用，特别是氧化石墨烯限域的π共轭结构对构建发光碳材料提供了十分便利的条件。目前，有大量的研究工作报道了氧化石墨烯及其衍生物能够产生多种颜色的荧光信号，然而，系统地总结这些研究去揭示氧化石墨烯发光机理的相关工作还比较少。本文总结了关于发光氧化石墨烯纳米材料的合成及其在光学成像方面应用的大量研究工作，为进一步开发新型的发光氧化石墨烯材料提供一些建设性意见。Abstract: As an opened-bandgap derivative, graphene oxide greatly enriches its optical properties and extends its applications in sensing and imaging. In particular, graphene oxide-confined π-conjugated structures provide very favorable conditions for the construction of luminescent carbon materials. Nowadays, more and more works have reported that graphene oxide and its derivatives can generate multicolor fluorescent signals. However, systematically summarizing these studies to reveal the luminescence mechanism of graphene oxide are still relatively rare. In this paper, the synthesis of luminescent graphene oxide nanomaterials and their application in optical imaging are summarized, which provides some constructive suggestions for the further development of new luminescent graphene oxide materials.
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Key words:
- graphene oxide /
- nanosheets /
- quantum dots /
- fluorescence /
- optical imaging
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图 1 (A) NGO-PEG与anti-CD20抗体(利妥昔单抗)选择性的结合及其细胞成像示意图[31]；(B)用NGO-PEG-Rituxan复合物处理CD20阳性表达的B淋巴细胞的NIR荧光图像[31]；(C)用NGO-PEG-Rituxan复合物处理CD20阴性表达的人T细胞白血病细胞的NIR荧光图像[31]；(D)GO胶体的紫外吸收和荧光发射光谱(插图：365 nm激发GO胶体的发光图像)[34]；(E)石墨烯样品被氧化5秒后在473 nm激发光激发下的共聚焦荧光图像。有意地进行强激光照射从而产生光漂白现象，如位置3所示[36]
Figure 1. (A)A schematic drawing illustrating the selective binding and cellular imaging of NGO-PEG conjugated with anti-CD20 antibody(Rituxan)[31]; (B)NIR fluorescence image of CD20 positive Raji B-cells treated with the NGO-PEG-Rituxan conjugate[31]; (C)NIR fluorescence image of CD20 negative CEM T-Cells treated with NGO-PEG-Rituxan conjugate[31]; (D)Typical absorption and fluorescence emission spectra of the as-prepared GO colloid(inset:photograph for GO colloids excited by 365 nm)[34]; (E)Confocal PL image excited at 473 nm for a graphene sample oxidized for 5 s. PL at position 3 is bleached intentionally by intense laser irradiation[36]
图 3 (A) GO和介孔二氧化硅薄膜的全固态荧光源示意图[49]。(B)通过在1200 s范围内调整直流偏置电压进而得到不同的PL光谱[50]。(C)对氧化石墨烯悬浮液进行在不同曝光时间(0~180 min)光热还原处理后的荧光光谱图[51]。(D)氧化石墨烯纳米片在365 nm紫外灯照射下荧光发射图[53]
Figure 3. (A)Schematic illustration of all-solid-state PL source made of GO and mesoporous SiO2 thin film[49]. (B)DC bias dependence of normalized PL spectra tuned by application of various DC bias voltages for 1 200 s[50]. (C)Normalized PL spectra of the GO suspensions after different exposure times(0~180 min) to photothermal reduction treatment[51]. (D)Photographs of the as-prepared luminescent GO nanosheets under 365 nm UV lamp irradiations[53]
图 4 (A) 利用水热法将GO切割成GQDs的机制及其荧光光谱[59]；(B)氨基功能化的GQDs的制备程序示意图及其荧光光谱图像[62]
Figure 4. (A)Mechanism for the hydrothermal cutting of GO sheets into GQDs and its photoluminescent spectra[59]; (B)schematic illustration of the preparative strategy for amino-functionalized GQDs, and the emission images as well as their photoluminescence spectra[62]
图 5 (A) GO纳米片的photo-Fenton反应原理示意图[65]; (B)碳纤维氧化切割成GQDs示意图[66]; (C)b-GQDs的合成示意图，含氧的位置有红色标记[67](彩图见电子版)
Figure 5. (A)Schematic representation of a proposed mechanism for the photo-Fenton reaction of the GO sheets[65]. (B)Representation scheme of oxidation cutting of carbon fiber into GQDs[66]. (C)Schematic illustration of the synthesis of b-GQDs. Oxygenated sites are shown in red[67](colour figures are available in electro-version)
图 6 (A) 将GQD与神经生长因子(NGF)结合的示意图[82]; (B)分子结构的GO与转铁蛋白和PEG结合的示意图[77]; (C)GO与分子染料FITC的体外双光子发光比较[76](彩图见电子版)
Figure 6. (A)Schematic illustration of conjugating a GQD with nerve growth factor(NGF)[82]; (B)a representation of the molecular structure of GO conjugated with transferrin and PEG[77]; (C)comparison of in vitro two-photon luminescence of GO with molecular dye FITC[76](color figures are available in electro-version)
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