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设计吡啶修饰的两亲性聚合物配体:提高水溶性胶体量子点的光学性能的更好的钝化。

Design of pyridyl-modified amphiphilic polymeric ligands: Towards better passivation of water-soluble colloidal quantum dots for improved optical performance.

机构信息

CIC biomaGUNE, Paseo Miramón, 182. Ed. C, 20009 San Sebastian, Spain.

CIC biomaGUNE, Paseo Miramón, 182. Ed. C, 20009 San Sebastian, Spain; Department of Physics, Philipps University of Marburg, Renthof 7, 35037 Marburg, Germany.

出版信息

J Colloid Interface Sci. 2016 Sep 15;478:88-96. doi: 10.1016/j.jcis.2016.05.058. Epub 2016 May 28.

DOI:10.1016/j.jcis.2016.05.058
PMID:27288574
Abstract

HYPOTHESIS

An effective surface passivation is crucial to obtain quantum dots (QDs) with good photoluminescence response. Whereas the encapsulation of QDs inside amphiphilic polymers provides colloidal stability, a decrease in the quantum yield (QY) is observed. Pyridyl motifs are known to bind strongly to the ZnS on core/shell QD and increase the structure rigidity. Hence, the incorporation of pyridyl groups into the polymer could make it more compact in order to improve the optical behavior of the QDs.

EXPERIMENTS

Pyridyl-modified amphiphilic polymeric ligands were synthesized based on a poly(isobutylene-alt-maleic anhydride) backbone with pyridyl and alkyl end-groups as anchoring groups. The proportion of both ligands was optimized. The resulting QDs were characterized using complementary techniques such as absorption spectroscopy, static and time-resolved photoluminescence spectroscopy, transmission electron microscopy, and dynamic light scattering.

FINDINGS

Coating with the designed polymer maintains the high QY of the QDs after being transferred to water and provides them colloidal stability under relevant biological conditions (i.e. wide range of pH and ionic strength, biological buffers and stability over time). The significant improvements of such ligand may be attributed to the synergistic effect of two anchoring groups (pyridyl and alkyl groups) which establish different types of interaction with the QD.

摘要

假设

获得具有良好光致发光响应的量子点(QD),有效的表面钝化至关重要。虽然将 QD 封装在两亲聚合物内部可以提供胶体稳定性,但量子产率(QY)会降低。已知吡啶基可以与核/壳 QD 的 ZnS 强结合,并增加结构刚性。因此,将吡啶基团引入聚合物中可以使其更加紧凑,从而改善 QD 的光学性能。

实验

基于聚(异丁烯-alt-马来酸酐)主链,合成了吡啶修饰的两亲性聚合物配体,吡啶基和烷基端基作为锚固基团。优化了两种配体的比例。使用互补技术,如吸收光谱、静态和时间分辨光致发光光谱、透射电子显微镜和动态光散射对所得 QD 进行了表征。

发现

设计的聚合物在转移到水中后仍能保持 QD 的高 QY,并在相关的生物条件下(即宽 pH 和离子强度范围、生物缓冲液和随时间的稳定性)提供胶体稳定性。这种配体的显著改进可能归因于两种锚固基团(吡啶基和烷基基团)的协同作用,它们与 QD 建立了不同类型的相互作用。

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