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WIREs Nanomed Nanobiotechnol

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Radiolabeling strategies and pharmacokinetic studies for metal based nanotheranostics

Advanced Review

Xiankai Sun, Yaowu Hao, Anil Pillai, Dianbo Zhang, Cheng‐Yang Wu, Ryan Hart, Aditi Mulgaonkar, Shahab Ranjbar Bahadori

Published Online: Oct 12 2020

DOI: 10.1002/wnan.1671

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Abstract Radiolabeled metal‐based nanoparticles (MNPs) have drawn considerable attention in the fields of nuclear medicine and molecular imaging, drug delivery, and radiation therapy, given the fact that they can be potentially used as diagnostic imaging and/or therapeutic agents, or even as theranostic combinations. Here, we present a systematic review on recent advances in the design and synthesis of MNPs with major focuses on their radiolabeling strategies and the determinants of their in vivo pharmacokinetics, and together how their intended applications would be impacted. For clarification, we categorize all reported radiolabeling strategies for MNPs into indirect and direct approaches. While indirect labeling simply refers to the use of bifunctional chelators or prosthetic groups conjugated to MNPs for post‐synthesis labeling with radionuclides, we found that many practical direct labeling methodologies have been developed to incorporate radionuclides into the MNP core without using extra reagents, including chemisorption, radiochemical doping, hadronic bombardment, encapsulation, and isotope or cation exchange. From the perspective of practical use, a few relevant examples are presented and discussed in terms of their pros and cons. We further reviewed the determinants of in vivo pharmacokinetic parameters of MNPs, including factors influencing their in vivo absorption, distribution, metabolism, and elimination, and discussed the challenges and opportunities in the development of radiolabeled MNPs for in vivo biomedical applications. Taken together, we believe the cumulative advancement summarized in this review would provide a general guidance in the field for design and synthesis of radiolabeled MNPs towards practical realization of their much desired theranostic capabilities. This article is categorized under: Nanotechnology Approaches to Biology > Nanoscale Systems in Biology Diagnostic Tools > Diagnostic Nanodevices Therapeutic Approaches and Drug Discovery > Nanomedicine for Oncologic Disease

Macrocyclic (upper) and acyclic (lower) bifunctional chelators for radiometal labeling of MNPs

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Substantially high tumoral retention was observed for the large sized ¹⁰³Pd/Pd‐coated hollow gold nanoshells (¹⁰³Pd/Pd‐HAuNPs) after intratumoral injection for brachytherapy application. (a) Simple schematic of ¹⁰³Pd/Pd‐HAuNPs synthesis through a Cu layer electrodeposition and subsequent Pd galvanic replacement and (b) SPECT/CT images of PC3‐tumor bearing SCID mice after 0, 1, 2, 4, 7, 14, 21, and 35 days of 1.51 mCi ¹⁰³Pd/Pd‐HAuNPs injection (Reprinted with permission from Moeendarbari et al. (2016). Copyright 2016 Nature Research)

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SPECT and fluorescence imaging evaluation of renal clearable ultrasmall glutathione‐coated‐[¹⁹⁸Au]AuNPs. SPECT images of Balb/c mice after (a) 10 min, (b) 1 hr, (c) 4 hr, and (d) 24 hr of injection with GS‐[¹⁹⁸Au]AuNPs and in vivo fluorescence imaging of (e) pre‐injection, (f) 5 min, (g) 20 min, (h) 1 hr, and (i) 24 hr GS‐[¹⁹⁸Au]AuNPs post‐injection (Reprinted with permission from C. Zhou et al. (2012). Copyright 2012 John Wiley and Sons)

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Tumor targeting capability of MNPs was achieved while retaining their renal clearance by tuning surface modification strategies. (a) PET/CT axial images depicting the accumulation of ⁶⁴Cu‐AMD3100, ⁶⁴Cu‐AuNCs‐AMD3100, and ⁶⁴Cu‐AuNCs radiotracers in 4T1 breast cancer tumor models after 1 week and 4 weeks of tumor implantation in mice, (b) quantitative 4T1 tumor uptake of the three treatments after 1, 2, 3, and 4 weeks of tumor implantation, and (c) tumor‐to‐muscle uptake ratios of the mentioned treatments after 1 week of tumor implantation (*p < .05, **p < .005, and ***p < .001) (Reprinted with permission from Y. Zhao, Detering, et al. (2016). Copyright 2016 American Chemical Society)

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(a) Schematic synthesis of MoS₂‐IO 2D nanocomposites by self‐assembly of meso‐2,3‐dimercaptosuccinnic acid (DMSA)‐modified IONPs on the MoS₂ nanosheets followed by PEGylation. (b) Radiolabeling of MoS₂‐IO‐(d)PEG with ⁶⁴Cu within the PEG layers (Reprinted with permission from T. Liu et al. (2015). Copyright 2015 American Chemical Society)

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Schematic synthesis of ¹²⁵I or ¹²⁴I‐encapsulated AuNPs (S. B. Lee et al., 2016)

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Comparative preparation of ⁵⁹Fe‐IONPs through (a) isotope exchange and (b) radiochemical doping techniques (Pospisilova et al., 2017)

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Schematic production of [¹³N]Al₂O₃ NPs by proton irradiation of Al₂O₃ NPs via the ¹⁶O(p,α)¹³N nuclear reaction (Reprinted with permission from Pérez‐Campaña et al. (2013). Copyright 2013 American Chemical Society)

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Schematic presentation of [email protected]₃O₄ NPs conjugation with DSPE‐PEG₂₀₀₀‐RGD and subsequent addition of Na¹²⁵I to synthesize the ¹²⁵I‐RGD‐PEG‐MNPs (Reprinted with permission from J. Wang, Zhao, et al. (2016). Copyright 2016 American Chemical Society)

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A schematic illustration of direct radiolabeling of AuNPs via homo‐radionuclide doping with ¹⁹⁹Au (Reprinted with permission from Chakravarty et al. (2018). Copyright 2018 American Chemical Society)

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Schematic synthesis of ⁶⁴Cu‐doped Au nanocages via co‐deposition of Au and Cu atoms on the pre‐synthesized Au nanocages and subsequent ⁶⁴Cu‐labeling through radiochemical doping technique (Reprinted with permission from M. Yang et al. (2017) with permission. Copyright 2016, John Wiley and Sons)

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(a) Schematic OVA and CpG lipid micelles presented on an IONP core directly labeled with ⁶⁷Ga and (b) microdosing of the nanosystem developed to deliver vaccine components to secondary lymphoid organs such as the lymph nodes (Reprinted with permission from Ruiz‐de‐Angulo et al. (2016). Copyright 2016 American Chemical Society)

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(a) Coating the IONPs with a layer of comb‐like oleylamine‐branched polyacrylic acid (COBP)‐NOTA, and (b) chelating ¹⁸F‐aluminum fluoride ions with NOTA on COBP‐NOTA functionalization of IONPs (Z. Sun et al., 2016)

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Schematic step‐wise synthesis of ⁶⁴Cu‐labeled AuNSs: (1) conjugating p‐NH₂‐Bn‐DOTA to OPSS‐PEG2k‐NHS, (2) coating the surface of AuNSs with OPSS‐PEG2k‐DOTA, (3) ⁶⁴Cu labeling of AuNS‐OPSS‐PEG2k‐DOTA, and (4) further pegylation with longer PEG5k‐thiol to shield the ⁶⁴Cu‐labeled AuNSs from external attacks (Reprinted with permission from H. Xie, Wang, et al. (2010). Copyright 2010 Elsevier)

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