Formation mechanism of carbon dots: From chemical structures to fluorescent behaviors

Despite the numerous reports on carbon dots (CDs) synthesized from o-phenylenediamine (o-pd), the precise mechanism of fluorescence and formation processes of o-pd CDs have not been investigated. In this study, we purified o-pd CDs and obtained five compounds with yellow, green and blue emission. For the first time, two actual molecular fluorophores named 2,3-Diaminophenazine (DAP) and 2-Amino-3-hydroxyphenazine (AHP) were confirmed. More sophisticated investigations showed the DAP was dominant for the yellow emission, which confirmed molecule states in detail. More interestingly, DAP could form nanoparticles (NPs) with various sizes at different concentrations. In this regard, we propose that the formation processes of o-pd CDs were similar to those of carbonized polymer dots (CPDs), where DAP structures initially aggregated with themselves to form polymeric clusters, further carbonization of polymeric clusters endowed the polymer clusters with a preliminary core-shell structure. With the collapse of the shell and aromatization of the core, the CPDs like structure formed eventually. This study supplements those on the yellow-emissive fluorophores region and could be the potential reference for the preparation of CDs in a similar system. Two fluorophores corresponded to yellow emission named DAP and AHP were separated from o-pd CDs solution by HPLC for the first time, further investigation suggested these CDs formed from the aggregation of DAP. [Display omitted] •The chemical structure of DAP and AHP were confirmed for the first time.•The blank of yellow-emissive fluorophores was supplemented.•The existence of molecule state prepared by rigid precursor was first verified.•The formation of CDs was originated from DAP.•The multi-colors LEDs with high CRI were successfully prepared by fluorophores.