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      Ferrimagnetic mPEG- b-PHEP copolymer micelles loaded with iron oxide nanocubes and emodin for enhanced magnetic hyperthermia–chemotherapy

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          Abstract

          As a non-invasive therapeutic method without penetration-depth limitation, magnetic hyperthermia therapy (MHT) under alternating magnetic field (AMF) is a clinically promising thermal therapy. However, the poor heating conversion efficiency and lack of stimulus–response obstruct the clinical application of magnetofluid-mediated MHT. Here, we develop a ferrimagnetic polyethylene glycol-poly(2-hexoxy-2-oxo-1,3,2-dioxaphospholane) (mPEG- b-PHEP) copolymer micelle loaded with hydrophobic iron oxide nanocubes and emodin (denoted as EMM). Besides an enhanced magnetic resonance (MR) contrast ability ( r 2 = 271 mM −1 s −1) due to the high magnetization, the specific absorption rate (2518 W/g at 35 kA/m) and intrinsic loss power (6.5 nHm 2/kg) of EMM are dozens of times higher than the clinically available iron oxide nanoagents (Feridex and Resovist), indicating the high heating conversion efficiency. Furthermore, this composite micelle with a flowable core exhibits a rapid response to magnetic hyperthermia, leading to an AMF-activated supersensitive drug release. With the high magnetic response, thermal sensitivity and magnetic targeting, this supersensitive ferrimagnetic nanocomposite realizes an above 70% tumor cell killing effect at an extremely low dosage (10 μg Fe/mL), and the tumors on mice are completely eliminated after the combined MHT–chemotherapy.

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          Nanotechnology for Multimodal Synergistic Cancer Therapy.

          The complexity, diversity, and heterogeneity of tumors seriously undermine the therapeutic potential of treatment. Therefore, the current trend in clinical research has gradually shifted from a focus on monotherapy to combination therapy for enhanced treatment efficacy. More importantly, the cooperative enhancement interactions between several types of monotherapy contribute to the naissance of multimodal synergistic therapy, which results in remarkable superadditive (namely "1 + 1 > 2") effects, stronger than any single therapy or their theoretical combination. In this review, state-of-the-art studies concerning recent advances in nanotechnology-mediated multimodal synergistic therapy will be systematically discussed, with an emphasis on the construction of multifunctional nanomaterials for realizing bimodal and trimodal synergistic therapy as well as the intensive exploration of the underlying synergistic mechanisms for explaining the significant improvements in synergistic therapeutic outcome. Furthermore, the featured applications of multimodal synergistic therapy in overcoming tumor multidrug resistance, hypoxia, and metastasis will also be discussed in detail, which may provide new ways for the efficient regression and even elimination of drug resistant, hypoxic solid, or distant metastatic tumors. Finally, some design tips for multifunctional nanomaterials and an outlook on the future development of multimodal synergistic therapy will be provided, highlighting key scientific issues and technical challenges and requiring remediation to accelerate clinical translation.
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            Multifunctional magnetic nanoparticles: design, synthesis, and biomedical applications.

            The combination of nanotechnology and molecular biology has developed into an emerging research area: nanobiotechnology. Magnetic nanoparticles are well-established nanomaterials that offer controlled size, ability to be manipulated externally, and enhancement of contrast in magnetic resonance imaging (MRI). As a result, these nanoparticles could have many applications in biology and medicine, including protein purification, drug delivery, and medical imaging. Because of the potential benefits of multimodal functionality in biomedical applications, researchers would like to design and fabricate multifunctional magnetic nanoparticles. Currently, there are two strategies to fabricate magnetic nanoparticle-based multifunctional nanostructures. The first, molecular functionalization, involves attaching antibodies, proteins, and dyes to the magnetic nanoparticles. The other method integrates the magnetic nanoparticles with other functional nanocomponents, such as quantum dots (QDs) or metallic nanoparticles. Because they can exhibit several features synergistically and deliver more than one function simultaneously, such multifunctional magnetic nanoparticles could have unique advantages in biomedical applications. In this Account, we review examples of the design and biomedical application of multifunctional magnetic nanoparticles. After their conjugation with proper ligands, antibodies, or proteins, the biofunctional magnetic nanoparticles exhibit highly selective binding. These results indicate that such nanoparticles could be applied to biological medical problems such as protein purification, bacterial detection, and toxin decorporation. The hybrid nanostructures, which combine magnetic nanoparticles with other nanocomponents, exhibit paramagnetism alongside features such as fluorescence or enhanced optical contrast. Such structures could provide a platform for enhanced medical imaging and controlled drug delivery. We expect that the combination of unique structural characteristics and integrated functions of multicomponent magnetic nanoparticles will attract increasing research interest and could lead to new opportunities in nanomedicine.
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              Magnetic nanomaterials for hyperthermia-based therapy and controlled drug delivery.

              Previous attempts to review the literature on magnetic nanomaterials for hyperthermia-based therapy focused primarily on magnetic fluid hyperthermia (MFH) using mono metallic/metal oxide nanoparticles. The term "hyperthermia" in the literature was also confined only to include use of heat for therapeutic applications. Recently, there have been a number of publications demonstrating magnetic nanoparticle-based hyperthermia to generate local heat resulting in the release of drugs either bound to the magnetic nanoparticle or encapsulated within polymeric matrices. In this review article, we present a case for broadening the meaning of the term "hyperthermia" by including thermotherapy as well as magnetically modulated controlled drug delivery. We provide a classification for controlled drug delivery using hyperthermia: Hyperthermia-based controlled drug delivery through bond breaking (DBB) and hyperthermia-based controlled drug delivery through enhanced permeability (DEP). The review also covers, for the first time, core-shell type magnetic nanomaterials, especially nanoshells prepared using layer-by-layer self-assembly, for the application of hyperthermia-based therapy and controlled drug delivery. The highlight of the review article is to portray potential opportunities for the combination of hyperthermia-based therapy and controlled drug release paradigms--towards successful application in personalized medicine. Copyright © 2011 Elsevier B.V. All rights reserved.
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                Author and article information

                Journal
                Natl Sci Rev
                Natl Sci Rev
                nsr
                National Science Review
                Oxford University Press
                2095-5138
                2053-714X
                April 2020
                17 January 2020
                17 January 2020
                : 7
                : 4
                : 723-736
                Affiliations
                [1 ] Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Key Laboratory of Metabolism and Regulation for Major Diseases of Anhui Higher Education Institutes, Hefei University of Technology , Hefei 230009, China
                [2 ] Institutes for Life Sciences, School of Medicine, South China University of Technology , Guangzhou 510006, China
                [3 ] Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, University of Science and Technology of China , Hefei 230026, China
                [4 ] Zhejiang Province Key Laboratory of Anti-Cancer Drug Research, College of Pharmaceutical Sciences, Key Laboratory of Biomedical Engineering of the Ministry of Education, Zhejiang University , Hangzhou 310058, China
                Author notes
                Corresponding author. E-mail: yanglu@ 123456hfut.edu.cn
                Corresponding author. E-mail: yangxz@ 123456scut.edu.cn
                Corresponding author. E-mail: shyu@ 123456ustc.edu.cn

                Equally contributed to this work.

                Author information
                http://orcid.org/0000-0003-3732-1011
                Article
                nwz201
                10.1093/nsr/nwz201
                8289054
                34692091
                c318aa2a-5f22-4663-8d10-bd6fad61b914
                © The Author(s) 2020. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.

                This is an Open Access article distributed under the terms of the Creative Commons Attribution License ( http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse, distribution, and reproduction in any medium, provided the original work is properly cited.

                History
                : 18 September 2019
                : 18 November 2019
                : 02 December 2019
                Page count
                Pages: 14
                Funding
                Funded by: National Natural Science Foundation of China, DOI 10.13039/501100001809;
                Award ID: 51572067
                Award ID: 51972090
                Award ID: 21501039
                Award ID: 51732011
                Award ID: 21431006
                Award ID: 21761132008
                Award ID: 51702309
                Award ID: 51822302
                Funded by: National Natural Science Foundation of China, DOI 10.13039/501100001809;
                Award ID: 21521001
                Funded by: Open Project of Key Laboratory of Biomedical Engineering of Guangdong Province;
                Award ID: KLBEMGD201903
                Funded by: National Basic Research Program of China, DOI 10.13039/501100012166;
                Award ID: 2014CB931800
                Funded by: Fundamental Research Funds for the Central Universities, DOI 10.13039/501100012226;
                Award ID: JZ2018HGPA0269
                Funded by: Natural Science Foundation of Anhui Province, DOI 10.13039/501100003995;
                Award ID: 1708085ME114
                Funded by: Major/Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology;
                Award ID: 2016FXZY005
                Categories
                Commentary
                Molecular Biology & Genetics
                AcademicSubjects/MED00010
                AcademicSubjects/SCI00010

                magnetic hyperthermia therapy,sensitive thermal response,chemotherapy,magnetic targeting,theranostics

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