Citation: WANG Yun-Jing, LIU Ying-Qiu, GAO Xiu-Xiu, ZHAN Yan-Shan, PAN Li-Yang, ZHANG Wen-Kai, FANG Xiao-Min. Surface Defect Passivation of Graphene Quantum Dots by Amino Functionalization and Photoluminescence Emission Enhancement[J]. Acta Physico-Chimica Sinica, ;2016, 32(10): 2636-2644. doi: 10.3866/PKU.WHXB201606282 shu

Surface Defect Passivation of Graphene Quantum Dots by Amino Functionalization and Photoluminescence Emission Enhancement

Henan Engineering Laboratory of Flame-Retardant and Functional Materials, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, Henan Province, P. R. China

Received Date: 24 May 2016
Revised Date: 24 June 2016

Fund Project: The project was supported by the National Natural Science Foundation of China (51403051, 21502042) and Key Project of the Education Department of Henan Province, China (16A150003).

In this work, graphene oxide sheets are cut into graphene quantum dots (GQDs) by acidic oxidation, then GQDs are hydrothermally treated with ammonia (NH₃) at 100℃ to form amino-functionalized graphene quantum dots (N-GQDs). Atomic force microscopy (AFM) shows smaller dots in ammonia treated GQDs, and holey graphene structure is directly observed. Fourier transform infrared (FTIR) spectra confirm that NH₃ can effectively react with epoxy and carboxyl groups to form hydroxylamine and amide groups, respectively. The absorption and photoluminescence (PL) properties of the samples are determined by ultraviolet-visible-near infrared (UV-Vis-NIR) spectra and steady-state fluorescence spectra. Three PL excitation peaks occurring at around 250, 290, and 350 nm are attributed to C=C related π-π^* transition, C-O-C and C=O related n-π^* transitions, respectively. After amino functionalization, the C-O-C related n-π^* transition is suppressed, and the PL emission spectrum of N-GQDs is less excitation wavelength. The fluorescence quantum yield of the N-GQDs is 9.6%, which is enhanced by 32 times compared with that of the unmodified GQDs (~0.3%). Timeresolved PL spectra are also used to investigate the N-GQDs. The PL lifetimes depend on the emission wavelength and coincide with the PL spectrum, and are different from most fluorescent species. This result reveals the synergy and competition between defect derived photoluminescence and amino passivation of the N-GQDs. Compared with oxygen-related defects, nitrogen-related localized electronic states are expected to have a longer lifetime and enhanced radiative decay rates.
- Graphene quantum dot,
- Photoluminescence,
- Amino,
- Defect,
- Passivation,
- Functionalization
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