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A multifunctional PHPMA-derived polymer for ratiometric pH sensing, fluorescence imaging and magnetic resonance imaging Fengyu Su, Shubhangi Agarwal, Tingting Pan, Yuan Qiao, Liqiang Zhang, Zhengwei Shi, Xiangxing Kong, Kevin Day, Meiwan Chen, Deirdre R. Meldrum, Vikram D Kodibagkar, and Yanqing Tian ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.7b15796 • Publication Date (Web): 06 Dec 2017 Downloaded from http://pubs.acs.org on December 6, 2017
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ACS Applied Materials & Interfaces
A multifunctional PHPMA-derived polymer for ratiometric pH sensing, fluorescence imaging and magnetic resonance imaging
Fengyu Sua,#, Shubhangi Agarwalb,#, Tingting Panc,d,#, Yuan Qiaoc, Liqiang Zhanga, Zhengwei Shia ， Xiangxing Konga, Kevin Daya ，Meiwan Chend, Deirdre Meldruma*, Vikram Kodibagkarb*, Yanqing Tianc*
a
Center for Biosignatures Discovery Automation, Biodesign Institute, Arizona State University, Tempe
85287, USA b
School for Biological and Health Systems Engineering, Arizona State University, Tempe AZ 85281,
USA c
Department of Materials Science and Engineering, Southern University of Science and Technology,
Shenzhen, Guangdong 518055, China d
State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences,
University of Macau, Avenida da Universidade, Taipa, Macau, China #:
These authors contribute equally
KEYWORDS: polymer, pH sensor, ratiometric sensor, MRI, fluorescence imaging, dual-modality
Abstract In this paper we report synthesis and characterization of a novel multi-modality (MRI/Fluorescence) probe for pH sensing and imaging. A multifunctional polymer was derived from poly(N-(2hydroxypropyl) methacrylamide) (PHPMA) and integrated with a naphthalimide-based-ratiometric fluorescence probe and a gadolinium-1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid complex (Gd-DOTA complex). The polymer was characterized using UV-vis absorption spectrophotometer, 1
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fluorescence spectrofluophotometer, magnetic resonance imaging (MRI), and confocal microscopy for optical and MRI-based pH sensing, and cellular imaging. In-vitro labeling of macrophage J774 and esophageal CP-A cell lines show the polymer’s ability to be internalized in the cells. The transverse relaxation time (T2) of the polymer was observed to be pH dependent while the spin-lattice relaxation time (T1) was not. The pH probe in the polymer shows strong fluorescence-based ratiometric pH response with emission window changes exhibiting blue emission under acidic conditions and green emission under basic conditions, respectively. This study provides new materials with multi-modalities for pH sensing and imaging.
Introduction Cellular pH (intra- and extra-cellular) plays a critical role in cellular metabolism, immune function, cell metastasis, and calcium signaling. Intracellular pH is heterogeneous due to the different functions of the various organelles, ranging from 4.5 in lysosome to 8.5 in mitochondria with an average around 7.41,2.The heterogeneity of pH in organelles, cells, tissues, and organs is critical in maintaining cell functions and pH homeostasis andcellular pH alterations are indicative of cell function changes and pathologies such as ischemia, chronic obstructive pulmonary disease, renal failure and cancer3. Extracellular pH is normally neutral around 7.2 and both intra and extra cellular pH regulate the function of each other. Low extracellular pH (
