Nanospace-confined preparation of uniform nitrogen-doped graphene quantum dots for highly selective fluorescence dual-function determination of Fe3+ and ascorbic acid

Abstract

N-Doped graphene quantum dots (N-GQDs) combine the advantages of N-doped carbon and quantum dot materials, displaying enhanced performance in electrocatalysis, drug delivery, sensing and so on. In this work, novel hydrotropic N-GQDs with controlled size are obtained for the first time via a nanospace-confined preparation strategy, in which HNO₃ vapour serves as scissors for quickly cutting the N-doped carbon nanolayer in the confined nanospace of reusable mesoporous molecular sieves. The as-prepared N-GQDs exhibit a uniform lateral size of about 2.4 nm, high photostability and yellow fluorescence, which is strongly quenched upon addition of ferric ions due to the coordination between ferric ions and N/O-rich groups of the N-GQDs surface. Significantly, the fluorescence response to Fe³⁺ is linear in the 0.5 to 40 μM concentration range and the N-GQDs showed good selectivity and satisfying recovery for ferric ion detection in tap water. Noteworthily, the quenched fluorescence by Fe³⁺ can be recovered by adding ascorbic acid (AA), which efficiently destroyed the coordination between Fe³⁺ and N-GQDs. Based on this principle, the N-GQDs were used to successfully construct an AA sensor, exhibiting a wide linearity range (between 0.5 and 90 μM) with a low detection of limit (80 nM at S/N = 3) and better selectivity towards AA compared with other common physiological substances. Finally, the constructed fluorescence sensor was employed successfully for AA determination in fish blood with satisfactory recovery ranging from 95.3 to 106.2%. The results indicate that N-GQDs synthesized by the nanospace-confined strategy are promising in biosensor fabrication.