The Formation Mechanism of Carbonized Polymer Dots: Crosslinking‐Induced Nucleation and Carbonization

作者：Chunlei Xia, Jundong Zhong, Xiao Han, Shoujun Zhu, Yunfeng Li, Hong Liu, Bai Yang · 发表于：Angewandte Chemie International Edition · 年份：2024 · DOI：10.1002/anie.202410519 · 被引用次数：80 · 研究领域：Pickering emulsions and particle stabilization、Carbon and Quantum Dots Applications、Covalent Organic Framework Applications

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.