文献类型：期刊文献

英文题名：Forster Resonance Energy Transfer Switchable Self-Assembled Micellar Nanoprobe: Ratiometric Fluorescent Trapping of Endogenous H2S Generation via Fluvastatin-Stimulated Upregulation

作者：Zhao, Chunchang[1,2];Zhang, Xiuli[1,2];Li, Kaibin[1,2];Zhu, Shaojia[3];Guo, Zhiqian[1,2];Zhang, Lili[1,2];Wang, Feiyi[1,2];Fei, Qiang[1,2];Luo, Sihang[1,2];Shi, Ping[3];Tian, He[1,2];Zhu, Wei-Hong[1,2]

机构：[1]E China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Collaborat Innovat Ctr Coal Based Energy i CCE, Shanghai Key Lab Funct Mat Chem, Inst Fine Chem, Shanghai 200237, Peoples R China;[3]E China Univ Sci & Technol, State Key Lab Bioreactor Engn, Shanghai 200237, Peoples R China

年份：2015

卷号：137

期号：26

起止页码：8490

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000357964400034)】；

基金：We gratefully acknowledge the financial support by National 973 Program (2013CB733700), NSFC for Creative Research Groups (21421004) and Distinguished Young Scholars (21325625), NSFC/China, the Oriental Scholarship, the Fundamental Research Funds for the Central Universities (WJ1416005), Science and Technology Commission of Shanghai Municipality (15XD1501400), and Shanghai Scientific and Technological Innovation Project (14520720700).

语种：英文

摘要：H2S produced in small amounts by mammalian cells has been identified in mediating biological signaling functions. However, the in situ trapping of endogenous H2S generation is still handicapped by a lack of straightforward methods with high selectivity and fast response. Here, we encapsulate a semi-cyanine-BODIPY hybrid dye (BODInD-Cl) and its complementary energy donor (BODIPY1) into the hydrophobic interior of an amphiphilic copolymer (mPEG-DSPE), especially for building up a ratiometric fluorescent H2S nanoprobe with extraordinarily fast response. A remarkable red-shift in the absorption band with a gap of 200 nm in the H2S response can efficiently switch off the Forster resonance energy transfer (FRET) from BODIPY1 to BODInD-Cl, subsequently recovering the donor fluorescence. Impressively, both the interior hydrophobicity of supramolecular micelles and electron-withdrawing nature of indolium unit in BODInD-Cl can sharply increase aromatic nudeophilic substitution with H2S. The ratiometric strategy based on the unique self-assembled micellar aggregate NanoBODIPY achieves an extremely fast response, enabling in situ imaging of endogenous H2S production and mapping its physiological and pathological consequences. Moreover, the amphiphilic copolymer renders the micellar assembly biocompatible and soluble in aqueous solution. The established FRET-switchable macromolecular envelope around BODInD-Cl and BODIPY1 enables cellular uptake, and makes a breakthrough in the trapping of endogenous H2S generation within raw264.7 macrophages upon stimulation with fluvastatin. This study manifests that cystathione gamma-lyase (CSE) upregulation contributes to endogenous H2S generation in fluvastatin-stimulated macrophages, along with a correlation between CSE/H2S and activating Akt signaling pathway.