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Photoluminescence Mechanisms of Dual-Emission Fluorescent Silver Nanoclusters Fabricated by Human Hemoglobin Template: From Oxidation- and Aggregation-Induced Emission Enhancement to Targeted Drug Delivery and Cell Imaging Publisher



Shamsipur M1 ; Molaabasi F2, 5 ; Sarparast M6 ; Roshani E3 ; Vaezi Z3 ; Alipour M7 ; Molaei K2 ; Naderimanesh H3 ; Hosseinkhani S4
Authors
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Authors Affiliations
  1. 1. Department of Chemistry, Razi University, Zakariya Razi Blvd., Kermanshah, Iran
  2. 2. Department of Chemistry, Tarbiat Modares University, Al Ahmad Street, Tehran, Iran
  3. 3. Department of Nanobiotechnology/Biophysics, Tarbiat Modares University, Al Ahmad Street, Tehran, Iran
  4. 4. Department of Biochemistry, Tarbiat Modares University, Al Ahmad Street, Tehran, Iran
  5. 5. Department of Biomaterials and Tissue Engineering, Breast Cancer Research Center, Motamed Cancer Institute, ACECR, Gandhi Street, Tehran, Iran
  6. 6. Department of Chemistry, Michigan State University, East Lansing, 48824-1322, MI, United States
  7. 7. Department of Advanced Medical Sciences and Technologies, School of Medicine, Jahrom University of Medical Sciences, Jahrom, Iran

Source: ACS Sustainable Chemistry and Engineering Published:2018


Abstract

A novel fundamental understanding of the features of mechanism for the synthesis of luminescent silver nanoclusters (AgNCs) in human hemoglobin (Hb) as capping/reducing agents is presented based upon simultaneous size transition and fluorescence enhancement phenomena The interesting features consist of both NC core oxidation and aggregation-induced emission (AIE) attributed to ligand-to-metal charge transfer (LMCT) or ligand-to-metal-metal charge transfer (LMMCT) from Ag(I)-Hb complexes (through oxygen, nitrogen, and sulfur atoms of Hb residues donation to the Ag(I) ions) forming Ag(0)@Ag(I)-Hb core-shell NCs, the origin and consequence being a dual emission/single excitation nanosystem with large stocks shift and high quantum yield obtained even at high temperature which is a challenging subject, is not reported until now. The bioconjugation of hyaluronic acid (HA) onto surfaces of an Hb layer (HA/AgNCs) produced a biocompatible platform with a doxorubicin drug (DOX) as DOX/HA/AgNCs for specific imaging and delivery of DOX via an efficient targeting of CD44-overexpressing cancer cells, which lead to an increased inhibition of tumor cell growth. Additionally, the cell viability analysis illustrated that the developed nanocarriers significantly enhanced the DOX uptake in HeLa cancer cells compared to HUVEC and HNCF-PI 52 normal cells allowing a selective cytotoxicity to HeLa cells. The suggested LMCT/LMMCT mechanism for an emission source combined with such attractive properties as a simple one-pot, nontoxic, synthesis route, long lifetime, large Stocks shift, excellent aqueous stability and photostability, and easy functionalization capability with good cell viability provided the possibility for a AgNCs nanoprobe for use to better understand the nucleation and growth mechanisms via computational modeling techniques (e.g., DFT study) and also for fabrication of new nanoprobes for developing multifunctional applications in the biobased chemical and electrochemical fields and in in vivo research. Copyright © 2018 American Chemical Society.
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