Multicolored pH-tunable and activatable fluorescence nanoplatform responsive to physiologic pH stimuli.

Multicolored pH-tunable and activatable fluorescence nanoplatform responsive to physiologic pH stimuli.
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DOI:
10.1021/ja300176w
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发表时间:
2012-05-09
影响因子:
15
通讯作者:
Gao, Jinming
Gao, Jinming
中科院分区:
化学1区
文献类型:
--
作者:
Zhou, Kejin;Liu, Haoming;Zhang, Shanrong;Huang, Xiaonan;Wang, Yiguang;Huang, Gang;Sumer, Baran D.;Gao, Jinming

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具有多色发射的可调谐的超pH响应荧光纳米颗粒在各种生物学研究中具有高度价值,例如内吞运输、内体/溶酶体成熟和亚细胞器中的pH调节。微小的差异(例如,<1个pH单位),但在不同的内吞隔室内精细调节的生理pH对这种系统的设计提出了巨大的挑战。在此,我们报告了一个一般的策略,以生产pH值可调的,高度可激活的多色荧光纳米粒子使用常用的pH值不敏感的染料与发射波长从绿色到近红外范围。pH诱导的胶束化是ON(单聚体)和OFF(胶束)状态之间荧光活化的主要驱动力。在三种可能的光化学机制中,homo Förster共振能量转移(homo-FRET)被认为是最简单的策略,使超pH响应超过H-二聚体和光诱导电子转移(PeT)机制。基于这一认识,我们选择了几种具有小斯托克位移(<40 nm)的荧光团,并建立了一组具有宽发射范围(500-820 nm)和不同pH转变的多色纳米颗粒。每个纳米颗粒保持尖锐的pH响应(开/关<0.25 pH单位),相应的pH转变点在pH 5.2、6.4、6.9和7.2。将多色纳米颗粒与人H2009肺癌细胞的混合物孵育证明了内吞隔室内的纳米颗粒的顺序激活与其pH转变直接相关。这种多色,pH可调的纳米平台为许多重要的细胞生理过程的研究提供了许多令人兴奋的机会,如pH调节和亚细胞器的内吞运输。
Tunable, ultra-pH responsive fluorescent nanoparticles with multichromatic emissions are highly valuable in a variety of biological studies, such as endocytic trafficking, endosome/lysosome maturation, and pH regulation in subcellular organelles. Small differences (e.g., <1 pH unit) and yet finely regulated physiological pH inside different endocytic compartments present a huge challenge to the design of such a system. Herein, we report a general strategy to produce pH-tunable, highly activatable multicolored fluorescent nanoparticles using commonly available pH-insensitive dyes with emission wavelengths from green to near IR range. pH-induced micellization is the primary driving force of fluorescence activation between the ON (unimer) and OFF (micelle) states. Among three possible photochemical mechanisms, homo Förster resonance energy transfer (homo-FRET) was found to be the most facile strategy to render ultra-pH response over the H-dimer and photoinduced electron transfer (PeT) mechanisms. Based on this insight, we selected several fluorophores with small Stoke shifts (<40 nm) and established a panel of multicolored nanoparticles with wide emission range (500-820 nm) and different pH transitions. Each nanoparticle maintained the sharp pH response (ON/OFF <0.25 pH unit) with corresponding pH transition point at pH 5.2, 6.4, 6.9 and 7.2. Incubation of a mixture of multicolored nanoparticles with human H2009 lung cancer cells demonstrated sequential activation of the nanoparticles inside endocytic compartments directly correlating with their pH transitions. This multicolored, pH-tunable nanoplatform offers many exciting opportunities for the study of many important cell physiological processes such as pH regulation and endocytic trafficking of subcellular organelles.
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