Lu Siyu, Sui Laizhi, Wu Min, Zhu Shoujun, Yong Xue, Yang Bai
State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun 130012 China.
College of Chemistry and Molecular Engineering Zhengzhou University 100 Kexue Road Zhengzhou 450001 China.
Adv Sci (Weinh). 2018 Nov 13;6(2):1801192. doi: 10.1002/advs.201801192. eCollection 2019 Jan 23.
Carbonized polymer dots (CPDs) have great potential for bioimaging and biosensing owing to their low toxicity, low cost, resistance to photobleaching, and low environmental impact. Here, the hydrothermal condensation of biomolecules (l-serine and l-tryptophan) is used to vary the CPDs' inner structure from amorphous to lattice. A new type of carbon lattice CPD is thus demonstrated that is bright (the photoluminescence quantum yield (PLQY) is as high as 89.57%) and shows room-temperature ferromagnetism (RTFM), with the magnetic moment increasing from 0.0025 emu g in crosslinked polymer clusters to 0.021 emu g in the latticed sample. Hydrothermal synthesis at 300 °C leads to a distinct type of CPD with an obvious carbon lattice, which shows the highest PLQY and the greatest ferromagnetism. Then, the origin of the RTFM is examined in the CPDs via first-principles calculation, revealing that graphitic nitrogen triggers RTFM in CPDs. Moreover, a possible growth mechanism is suggested that includes kinetics as an important factor in the formation of the CPD crystallites. Overall, these findings identify graphitic nitrogen and high crystallinity as crucial to the enhancement of the CPDs' photoluminescence and room-temperature ferromagnetism which suggests that they deserve more research attention to develop practical applications.
碳化聚合物点(CPDs)因其低毒性、低成本、抗光漂白性和低环境影响,在生物成像和生物传感方面具有巨大潜力。在此,利用生物分子(L-丝氨酸和L-色氨酸)的水热缩合来改变CPDs的内部结构,使其从无定形变为晶格结构。由此展示了一种新型的碳晶格CPD,其发光明亮(光致发光量子产率(PLQY)高达89.57%)并表现出室温铁磁性(RTFM),磁矩从交联聚合物簇中的0.0025 emu g增加到晶格样品中的0.021 emu g。300℃的水热合成产生了一种具有明显碳晶格的独特CPD类型,其显示出最高的PLQY和最大的铁磁性。然后,通过第一性原理计算研究了CPDs中RTFM的起源,揭示了石墨氮引发了CPDs中的RTFM。此外,还提出了一种可能的生长机制,其中动力学是CPD微晶形成的重要因素。总体而言,这些发现表明石墨氮和高结晶度对于增强CPDs的光致发光和室温铁磁性至关重要,这表明它们值得更多的研究关注以开发实际应用。