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Langmuir. 2018 Jan 9;34(1):250-258. doi: 10.1021/acs.langmuir.7b03425. Epub 2017 Dec 28.

Electrochemical Cutting in Weak Aqueous Electrolytes: The Strategy for Efficient and Controllable Preparation of Graphene Quantum Dots.

Huang H1,2, Yang S1,2, Li Q1,2, Yang Y2,3, Wang G4, You X1,2, Mao B1,2, Wang H1,2, Ma Y1, He P1,2, Liu Z1,2,3, Ding G1,2, Xie X1,2,3.

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State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences , Shanghai 200050, P. R. China.
University of Chinese Academy of Sciences , Beijing 100049, P. R. China.
School of Physical Science and Technology, ShanghaiTech University , Shanghai 200031, P. R. China.
Department of Microelectronic Science and Engineering, Faculty of Science, Ningbo University , Ningbo 315211, P. R. China.


The controllable and efficient electrochemical preparation of highly crystalline graphene quantum dots (GQDs) in an aqueous system is still challenging. Here, we developed a weak electrolyte-based (typically an ammonia solution) electrochemical method to enhance the oxidation and cutting process and therefore achieve a high yield of GQDs. The yield of GQDs (3-8 nm) is 28%, approximately 28 times higher than the yield of GQDs prepared by other strong electrolytes. The whole preparation process can be accomplished within 2 h because of the effective free radical oxidation process and the suppressed intercalation-induced exfoliation in weakly ionized aqueous electrolytes. The GQDs also showed excellent crystallinity which is obviously better than the crystallinity of GQDs obtained via bottom-up approaches. Moreover, amino-functionalization of GQDs can be realized by manipulating the electrolyte concentration. We further demonstrate that the proposed method can also be expanded to other weak electrolytes (such as HF and H2S) and different anode precursor materials (such as graphene/graphite papers, carbon fibers, and carbon nanotubes).

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