Xia Chunlei, Zhong Jundong, Han Xiao, Zhu Shoujun, Li Yunfeng, Liu Hong, Yang Bai
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130012, P. R. China.
School of Environment, South China Normal University, Guangzhou Higher Education Mega Center, Panyu District, Guangzhou, 510006, P. R. China.
Angew Chem Int Ed Engl. 2024 Oct 24;63(44):e202410519. doi: 10.1002/anie.202410519. Epub 2024 Sep 17.
Carbon dots (CDs), as a kind of zero-dimensional nanomaterials, have been widely synthesized by bottom-up methods from various precursors. However, the formation mechanism is still unclear and controversial, which also brings difficulty to the regulation of structures and properties. Only some tentative formation processes were postulated by analyzing the products obtained at different reaction times and temperatures. Here, the effect of crosslinking on the formation of carbonized polymer dots (CPDs) is explored. Crosslinking-induced nucleation and carbonization (CINC) is proposed as the driving force for the formation of CPDs. Under hydrothermal synthesis, the precursors are initiated to polymerize and crosslink. The crosslinking brings higher hydrophobicity to generate the hydrophilic/hydrophobic microphase separation, which promotes dehydration and carbonization resulting in the formation of CPDs. Based on the principle of CINC, the influence factors of size are also revealed. Moreover, the dissipative particle dynamics (DPD) simulation is employed to support this formation mechanism. This concept of CINC will bring light to the formation process of CPDs, as well as facilitate the regulation of CPDs' size and photoluminescence.
碳点（CDs）作为一种零维纳米材料，已通过自下而上的方法从各种前驱体中广泛合成。然而，其形成机制仍不明确且存在争议，这也给结构和性能的调控带来了困难。仅通过分析在不同反应时间和温度下获得的产物，推测了一些初步的形成过程。在此，探索了交联对碳化聚合物点（CPDs）形成的影响。提出交联诱导成核与碳化（CINC）是CPDs形成的驱动力。在水热合成条件下，前驱体开始聚合和交联。交联带来更高的疏水性，从而产生亲水/疏水微相分离，这促进了脱水和碳化，导致CPDs的形成。基于CINC原理，还揭示了尺寸的影响因素。此外，采用耗散粒子动力学（DPD）模拟来支持这一形成机制。CINC这一概念将为CPDs的形成过程带来启示，并有助于调控CPDs的尺寸和光致发光性能。
