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WIREs Nanomed Nanobiotechnol
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Polymer‐based activatable optical probes for tumor fluorescence and photoacoustic imaging

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Abstract Optical imaging including fluorescence imaging and photoacoustic imaging have been widely employed in early and accurate diagnosis of cancer. Compared to the “always on” optical probes, the molecular probes that could emit their signal in response to the tumor microenvironment exhibit the low background noise and high signal‐to‐background ratio, allowing sensitive and accurate cancer diagnosis. Polymer‐based activatable optical probes display the advantages of improved water solubility, good photostability, extended blood circulation time, and easy functionalization, which enable them to accumulate in tumor for early and accurate diagnosis. This review focuses on recent advances in the development of polymer‐based activatable optical probes for tumor fluorescence and PA imaging. The designs of polymer‐based optical probes are first discussed. Then the applications for tumor fluorescence and PA imaging using pH, hypoxia, reactive oxygen and nitrogen species, and enzymes responsive polymer‐based optical probes are discussed in details. At last, the present challenges and perspectives of polymer‐based activatable optical probes to further advance them into the clinical application are also suggested. This article is categorized under: Diagnostic Tools > In vivo Nanodiagnostics and Imaging Diagnostic Tools > Biosensing
Schematic illustration of polymer‐based activatable optical probe for tumor fluorescence and PA imaging. PA, photoacoustic
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(a) Schematic illustration of the activation mechanism of CyGal‐P in βGal‐overexpressing cancer cells. (b) The fluorescence spectra and images of CyGal‐P in the absence or presence of βGal. (c) The PA spectra and images of CyGal‐P and CyGal in the absence or presence of βGal. (d and f) in vivo representative near infrared fluorescence (NIRF) (d) and PA (f) images of subcutaneous SKOV3 xenograft tumors in living mice before and after i.v. administration of CyGal‐P or CyGal. (e and g) Fluorescence intensities (e) and PA intensity increments (g) of tumor at different time points after i.v. injection of CyGal‐P or CyGal. (h) PA intensity increments spectra of tumors after i.v. injection of CyGal‐P and CyGal at 60 min. (i) Design and mechanism of the enzyme‐responsive self‐assembly optical probe 1 in TME that showed the AIR effect to enhance PA signals. (j) Representative PA images of tumors at different time points after injection with optical probes 1, 2, and 3 or PBS. (k) Quantification of PA signal intensity in tumors at different time points after injection with optical probes 1, 2, and 3 or phosphate buffered saline (PBS). (l) ex vivo quantification of the amounts of optical probes 1, 2, and 3 in tumors at 10 and 96 hr postinjection. (Figure [a–h] was reprinted with permission from X. Zhen et al. (). Copyright 2018 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). (Figure [i–l] was reprinted with permission from D. Zhang et al. (). Copyright 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). PA, photoacoustic; TME, tumor microenvironment
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(a) Schematic illustration of the design of the liposome‐based activatable PA nanoprobe (Lipo@HRP@ABTS). (b) The absorbance of nanoprobes at 800 nm after treatment with catalase and different types of RONS. The absorbance (c) and the PA signals (d) of nanoprobes at 800 nm after treatment with different concentrations of H2O2. (e) The representative in vivo PA images of subcutaneous 4T1 xenograft tumor at different time points after i.v. injection with nanoprobes. (f) PA signals in tumors based on PA imaging data shown in (e). (g) Schematic illustration of the preparation of organic semiconducting nanoprobes (OSNs) via nanoprecipitation. (h) The PA spectra of nanoprobe OSN‐B1 before and after addition of H2O2 or ONOO. (i) The representative in vivo PA images of subcutaneous 4T1 xenograft tumor in NAC‐treated and untreated mice after i.v. injection of nanoprobe OSN‐B1. (Figure [a–f] was reprinted with permission from Q. Chen et al. (). Copyright 2017 National Academy of Sciences). (Figure [g–i] was reprinted with permission from J. Zhang et al. (). Copyright 2017 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). NAC, N‐acetyl‐l‐cysteine; PA, photoacoustic; RONS, reactive oxygen and nitrogen species
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(a) Schematic illustration of the two‐step cascade signals amplification process of the probe to the acidic and hypoxic TME. (b) Chemical structure and preparation of nanoprobe Pt‐TPP‐PVP430. (c) Schematic illustration of the ratiometric hypoxia‐imaging mechanism of nanoprobe Pt‐TPP‐PVP430 in vivo. (Figure [a] was reprinted with permission from Zheng et al. (). Copyright 2017 Nature Publishing Group). (Figure [b and c] was reprinted with permission from S. Wang et al. (). Copyright 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). TME, tumor microenvironment
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(a) The structure of the ultra pH‐sensitive nanoprobes and schematic illustration of the mechanism of fluorescence imaging of tumor pH. (b) The response of UPSe and UPSi nanoprobes to the change of pH condition. (c) Representative in vivo fluorescent images of subcutaneous A549 xenograft tumor‐bearing mice at 24 hr after i.v. injection with UPSe nanoprobes and the controls. (d) The tumor‐to‐normal tissues fluorescence intensity ratio (T/N ratio) as a function of time after injection with nanoprobes. (e) Representative in vivo fluorescent images of subcutaneous A549 xenograft tumor‐bearing mice at 6 hr after i.v. injection with UPSi or cRGD‐UPSi nanoprobes. (f) T/N ratio as a function of time after injection with nanoprobes. (g) The structure of the PEGylated BODIPY probes with different PEG lengths. (h) Representative ex vivo bioluminescence and fluorescence images of harvested organs from pancreas and tibia cancer metastasis‐bearing mice (i and ii) and normal BL6 mice (iii) sacrificed at 24 hr after i.v. injection with PEG2K‐BODIPY. (i) T/S ratios of PEG2K‐BODIPY fluorescence intensity at 24 hr after i.v. injection. Statistical significance was determined using a two‐tailed Student's t test (***p ≤ .001; *p ≤ .05). (j) Representative ex vivo bioluminescence and fluorescence images of harvested organs from liver, lung, and kidney cancer metastasis‐bearing mice sacrificed at 24 hr after i.v. injection with PEG2K‐BODIPY. (k) T/S ratios of PEG2K‐BODIPY fluorescence intensity at 24 hr after i.v. injection. (Figure [a–f] was reprinted with permission from Y. Wang et al. (). Copyright 2014 Nature Publishing Group). (Figure [g–k] was reprinted with permission from Xiong et al. (). Copyright 2017 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). UPS, ultra pH‐sensitive nanoprobe
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(a) The schematic illustration of the preparation of HSA‐BPOx‐IR825 nanoprobe and its mechanism for ratiometric PA imaging of tumor pH. (b) The PA680/PA825 intensity ratios of HSA‐BPOx‐IR825 nanoprobe tested in different pH values. (c) Representative in vivo PA images of tumors with different sizes after systemic administration of HSA‐BPOx‐IR825 nanoprobe. (d) The PA680/PA825 intensity ratios and pH of tumors calculated based on PA signal intensity in (c). (e) Chemical structures of the SO (F‐DTS), the pH‐BDP, and PEG‐b‐PPG‐b‐PEG. (f) Schematic illustration of the ratiometric tumor pH PA imaging mechanism. (g) PA spectra of nanoprobe tested at different pH values. (h) The PA680/PA750 intensity ratios of nanoprobe tested at different pH values. (i) Representative in vivo PA images and ratiometric images (PA680/PA750) of HeLa tumor before and after 6 hr systemic administration of nanoprobe. (j) PA signals and ratiometric PA signals (PA680/PA750) as a function of time postinjection with nanoprobe. **No statistically significant difference in PA680/PA750 between 3 and 6 hr (p > .05, n = 3). (Figure [a–d] was reprinted with permission from Q. Chen et al. (). Copyright 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). (Figure [e–j] was reprinted with permission from Miao et al. (). Copyright 2016 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim). HAS, human serum albumin; PA, photoacoustic; SO, semiconducting oligomer
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Diagnostic Tools > In Vivo Nanodiagnostics and Imaging
Diagnostic Tools > Biosensing

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