Bai Yi-Yan, Yang Yan-Ju, Xu Ying, Yang Xiao-Yan, Zhang Zhi-Ling
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, People's Republic of China.
Department of Chemistry, Yuncheng University, Yuncheng 044000, People's Republic of China.
Anal Chem. 2023 Mar 7;95(9):4429-4434. doi: 10.1021/acs.analchem.2c05016. Epub 2023 Feb 22.
In situ monitoring of the agglomeration/aggregation process of nanoparticles (NPs) is crucial because it seriously affects cell entry, biosafety, catalytic performance of NPs, and so on. Nevertheless, it remains hard to monitor the solution phase agglomeration/aggregation of NPs via conventional techniques such as electron microscopy, which requires sample pretreatment and cannot represent native state NPs in solution. Considering that single-nanoparticle electrochemical collision (SNEC) is powerful to detect NPs in solution at the single-particle level, and the current lifetime, which refers to the time that current intensity decays to 1/e of the original value, is skilled in distinguishing different sized NPs, herein, a current lifetime-based SNEC has been developed to distinguish a single Au NP ( = 18 nm) from its agglomeration/aggregation. Based on this, the agglomeration/aggregation process of small-sized NPs and the discrimination of agglomeration vs aggregation have been carefully investigated at the single-particle level. Results showed that the agglomeration/aggregation of Au NPs ( = 18 nm) in 0.8 mM HClO climbed from 19% to 69% over two hours, whereas there was no visible granular sediment, and Au NPs tended to agglomerate rather than aggregate irreversibly under normal conditions. Hence, the proposed current lifetime-based SNEC could serve as a complementary method to in situ monitor the agglomeration/aggregation of small-sized NPs in solution at the single-particle level and provide effective guidance for the practical application of NPs.
对纳米颗粒(NPs)团聚/聚集过程进行原位监测至关重要,因为这会严重影响细胞摄取、生物安全性、NPs的催化性能等。然而,通过电子显微镜等传统技术来监测NPs在溶液相中的团聚/聚集仍然困难,这些技术需要对样品进行预处理,且无法呈现溶液中NPs的天然状态。鉴于单纳米颗粒电化学碰撞(SNEC)在单颗粒水平检测溶液中NPs方面具有强大功能,且电流寿命(即电流强度衰减至原始值的1/e 时所经历的时间)擅长区分不同尺寸的NPs,在此,已开发出一种基于电流寿命的SNEC来区分单个金纳米颗粒( = 18 nm)与其团聚/聚集状态。基于此,已在单颗粒水平上仔细研究了小尺寸NPs的团聚/聚集过程以及团聚与聚集的区分。结果表明,在0.8 mM HClO中,18 nm的金纳米颗粒的团聚/聚集在两小时内从19%攀升至69%,而没有可见的颗粒沉淀,并且在正常条件下金纳米颗粒倾向于团聚而非不可逆地聚集。因此,所提出的基于电流寿命的SNEC可作为一种补充方法,用于在单颗粒水平上原位监测溶液中小尺寸NPs的团聚/聚集,并为NPs的实际应用提供有效指导。