Publications by authors named "Xiangyang Shi"

284 Publications

Intelligent nanogels with self-adaptive responsiveness for improved tumor drug delivery and augmented chemotherapy.

Bioact Mater 2021 Oct 24;6(10):3473-3484. Epub 2021 Mar 24.

College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai, 201620, China.

For cancer nanomedicine, the main goal is to deliver therapeutic agents effectively to solid tumors. Here, we report the unique design of self-adaptive ultrafast charge-reversible chitosan-polypyrrole nanogels (CH-PPy NGs) for enhanced tumor delivery and augmented chemotherapy. CH was first grafted with PPy to form CH-PPy polymers that were used to form CH-PPy NGs through glutaraldehyde cross-linking a miniemulsion method. The CH-PPy NGs could be finely treated with an alkaline solution to generate ultrafast charge-reversible CH-PPy-OH-4 NGs (R-NGs) with a negative charge at a physiological pH and a positive charge at a slightly acidic pH. The R-NGs display good cytocompatibility, excellent protein resistance, and high doxorubicin (DOX) loading efficiency. Encouragingly, the prepared R-NGs/DOX have prolonged blood circulation time, enhanced tumor accumulation, penetration and tumor cell uptake due to their self-adaptive charge switching to be positively charged, and responsive drug delivery for augmented chemotherapy of ovarian carcinoma . Notably, the tumor accumulation of R-NGs/DOX (around 4.7%) is much higher than the average tumor accumulation of other nanocarriers (less than 1%) reported elsewhere. The developed self-adaptive PPy-grafted CH NGs represent one of the advanced designs of nanomedicine that could be used for augmented antitumor therapy with low side effects.
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http://dx.doi.org/10.1016/j.bioactmat.2021.03.021DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8024537PMC
October 2021

Core-Shell Tecto Dendrimers Enable Enhanced Tumor MR Imaging through an Amplified EPR Effect.

Biomacromolecules 2021 May 13;22(5):2181-2188. Epub 2021 Apr 13.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Shanghai Engineering Research Center of Nano-Biomaterials and Regenerative Medicine, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

Development of nanoplatforms that can amplify the passive tumor targeting effect based on enhanced permeability and retention (EPR) effect is crucial for precision cancer nanomedicine applications. Herein, we present the development of core-shell tecto dendrimers (CSTDs) as a platform for enhanced tumor magnetic resonance (MR) imaging through an amplified EPR effect. In this work, poly(amidoamine) (PAMAM) dendrimers of generation 5 (G5) were decorated with β-cyclodextrin (CD) and then assembled with G3 PAMAM dendrimers premodified with adamantane (Ad) via supramolecular recognition of CD and Ad. The formed G5-CD/Ad-G3 CSTDs were conjugated with tetraazacyclododecane tetraacetic acid (DOTA)-Gd(III) chelators and further acetylated to neutralize the remaining CSTD periphery amines. We reveal that the formed CSTD.NHAc-DOTA(Gd) (CSTD-D-Gd) complexes have a narrow size distribution and satisfactory colloidal stability, and are cytocompatible within the concentration range studied. Compared to the single dendrimer counterpart of G5.NHAc-DOTA(Gd) (G5-D-Gd) complexes, the CSTD-D-Gd complexes with a higher molecular weight and volume possess a longer rotation correlation time, hence having a longitudinal relaxivity () of 7.34 mM s, which is 1.5 times larger than that of G5-D-Gd complexes (4.92 mM s). More importantly, the CSTD-D-Gd complexes display better permeability in the three-dimensional (3D) cell spheroids through fluorescence imaging and a more significant EPR effect for improved tumor MR imaging than the G5-DOTA-Gd complexes. The generated CSTD-D-Gd complexes may be adopted for enhanced tumor MR imaging through an amplified passive EPR effect and also be further extended for different cancer theranostic applications.
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http://dx.doi.org/10.1021/acs.biomac.1c00262DOI Listing
May 2021

Dendrimer-decorated nanogels: Efficient nanocarriers for biodistribution and chemotherapy of ovarian carcinoma.

Bioact Mater 2021 Oct 13;6(10):3244-3253. Epub 2021 Mar 13.

DWI-Leibniz-Institute for Interactive Materials e.V, 52056, Aachen, Germany.

Nanomedicine has revolutionized disease theranostics by the accurate diagnosis and efficient therapy. Here, the PAMAM dendrimer decorated PVCL-GMA nanogels (NGs) were developed for favorable biodistribution and enhanced antitumor efficacy of ovarian carcinoma. By an ingenious design, the NGs with a unique structure that GMA-rich domains were localized on the surface were synthesized precipitation polymerization. After G2 dendrimer decoration, the overall charge is changed from neutral to positive, and the NGs-G2 display the whole charge nature of positively charged corona and neutral core. Importantly, the unique architecture and charge conversion of NGs-G2 have a profound impact on the biodistribution and drug delivery . As a consequence of this alteration, the NGs-G2 as nanocarriers emerge the highly sought biodistribution of reduced liver accumulation, enhanced tumor uptake, and promoted drug release, resulting in the significantly augmented antitumor efficacy with low side effects. Remarkably, this finding is contrary to some reported work that the nanocarriers with positive charge have preferential liver uptake. Moreover, the NGs-G2 also displayed thermal/pH dual-responsive behaviors, excellent biocompatibility, improved cellular uptake, and stimuli-responsive drug release. Encouragingly, this work demonstrates a novel insight into the strategy for optimizing design, improving biodistribution and enhancing theranostic efficacy of nanocarriers.
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http://dx.doi.org/10.1016/j.bioactmat.2021.02.031DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7970313PMC
October 2021

Comparison of the effects of dendrimer, micelle and silver nanoparticles on phospholipase A2 structure.

J Biotechnol 2021 Apr 13;331:48-52. Epub 2021 Mar 13.

Institute of Biophysics and Cell Engineering of NASB, Minsk, Belarus. Electronic address:

The interaction of nanoparticles (NP) with proteins (the so-called 'protein corona') is a huge challenge in attempting to apply them in personalized nanomedicine. We have analyzed the interaction between A) two 'soft' NPs (a cationic phosphorus dendrimer of generation 3; a cationic phosphorus amphiphilic dendron of generation 2), and B) one 'hard' nanoparticle (silver NP covered with cationic carbosilane dendritic moieties); and membrane-bound protein phospholipase A2 from bovine pancreas. The hard and soft NPs have differences in the nature of their interactions with phospholipase A2. This enzyme surrounds hard AgNP, whereas dendrimer and amphiphilic dendron form aggregates/micelles with phospholipase A2. There is a difference in action of phospholipase A2 bound to the core of dendrimer, and of micelles formed from non-covalent interactions between the amphiphilic dendron. These data are important in understanding the nature of interaction between different kinds of nanoparticles and proteins.
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http://dx.doi.org/10.1016/j.jbiotec.2021.03.009DOI Listing
April 2021

Engineered non-invasive functionalized dendrimer/dendron-entrapped/complexed gold nanoparticles as a novel class of theranostic (radio)pharmaceuticals in cancer therapy.

J Control Release 2021 Apr 4;332:346-366. Epub 2021 Mar 4.

Laboratoire de Chimie de Coordination du CNRS, 205 route de Narbonne, 31077 Toulouse Cedex 4, France; Université Toulouse 118 route de Narbonne, 31077 Toulouse Cedex 4, France. Electronic address:

Nanomedicine represents a very significant contribution in current cancer treatment; in addition to surgical intervention, radiation and chemotherapeutic agents that unfortunately also kill healthy cells, inducing highly deleterious and often life-threatening side effects in the patient. Of the numerous nanoparticles used against cancer, gold nanoparticles had been developed for therapeutic applications. Inter alia, a large variety of dendrimers, i.e. soft artificial macromolecules, have turned up as non-viral functional nanocarriers for entrapping drugs, imaging agents, and targeting molecules. This review will provide insights into the design, synthesis, functionalization, and development in biomedicine of engineered functionalized hybrid dendrimer-tangled gold nanoparticles in the domain of cancer theranostic. Several aspects are highlighted and discussed such as 1) dendrimer-entrapped gold(0) hybrid nanoparticles for the targeted imaging and treatment of cancer cells, 2) dendrimer encapsulating gold(0) nanoparticles (Au DENPs) for the delivery of genes, 3) Au DENPs for drug delivery applications, 4) dendrimer encapsulating gold radioactive nanoparticles for radiotherapy, and 5) dendrimer/dendron-complexed gold(III) nanoparticles as technologies to take down cancer cells.
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http://dx.doi.org/10.1016/j.jconrel.2021.03.003DOI Listing
April 2021

Correction: A polydopamine-coated LAPONITE®-stabilized iron oxide nanoplatform for targeted multimodal imaging-guided photothermal cancer therapy.

J Mater Chem B 2021 Mar;9(10):2549

State Key Laboratory of Modification of Chemical Fibers and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

Correction for 'A polydopamine-coated LAPONITE®-stabilized iron oxide nanoplatform for targeted multimodal imaging-guided photothermal cancer therapy' by Mengxue Liu et al., J. Mater. Chem. B, 2019, 7, 3856-3864, DOI: 10.1039/c9tb00398c.
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http://dx.doi.org/10.1039/d1tb90032cDOI Listing
March 2021

Recent developments of cancer nanomedicines based on ultrasmall iron oxide nanoparticles and nanoclusters.

Nanomedicine (Lond) 2021 04 4;16(8):609-612. Epub 2021 Mar 4.

State Key Laboratory for Modification of Chemical Fibers & Polymer Materials, International Joint Laboratory for Advanced Fiber & Low-dimension Materials, College of Chemistry, Chemical Engineering & Biotechnology, Donghua University, Shanghai 201620, PR China.

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http://dx.doi.org/10.2217/nnm-2021-0033DOI Listing
April 2021

Construction of Poly(amidoamine) Dendrimer/Carbon Dot Nanohybrids for Biomedical Applications.

Macromol Biosci 2021 Apr 22;21(4):e2100007. Epub 2021 Feb 22.

Key Laboratory of Science & Technology of Eco-Textile, Ministry of Education, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai, 201620, P. R. China.

Design of intelligent hybrid nanoparticles that can integrate diagnosis and therapy components plays an important role in the field of nanomedicine. Poly(amidoamine) (PAMAM) dendrimers possessing a unique architecture and tunable functional groups have been widely developed for various biomedical applications. Carbon dots (CDs) are considered as a promising fluorescence probe or drug delivery system due to their stable fluorescence property and excellent biocompatibility. The distinctive merits of PAMAM dendrimers and CDs are amenable for them to be constructed as perfect nanohybrids for different biomedical applications, in particular for cancer nanomedicine. Here, the recent advances in the construction of PAMAM dendrimer/CD nanohybrids for diverse biomedical applications, in particular for sensing and cancer theranostics are summarized. Finally, the future perspectives of the PAMAM dendrimer/CD nanohybrids are also briefly discussed.
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http://dx.doi.org/10.1002/mabi.202100007DOI Listing
April 2021

Polydopamine-Coated Laponite Nanoplatforms for Photoacoustic Imaging-Guided Chemo-Phototherapy of Breast Cancer.

Nanomaterials (Basel) 2021 Feb 4;11(2). Epub 2021 Feb 4.

College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, China.

Theranostic nanoplatforms combining photosensitizers and anticancer drugs have aroused wide interest due to the real-time photoacoustic (PA) imaging capability and improved therapeutic efficacy by the synergistic effect of chemotherapy and phototherapy. In this study, polydopamine (PDA) coated laponite (LAP) nanoplatforms were synthesized to efficiently load indocyanine green (ICG) and doxorubicin (DOX), and modified with polyethylene glycol-arginine-glycine-aspartic acid (PEG-RGD) for PA imaging-guided chemo-phototherapy of cancer cells overexpressing αβ integrin. The formed ICG/LAP-PDA-PEG-RGD/DOX nanoplatforms showed significantly higher photothermal conversion efficiency than ICG solution and excellent PA imaging capability, and could release DOX in a pH-sensitive and NIR laser-triggered way, which is highly desirable feature in precision chemotherapy. In addition, the ICG/LAP-PDA-PEG-RGD/DOX nanoplatforms could be uptake by cancer cells overexpressing αβ integrin with high specificity, and thus serve as a targeted contrast agent for in vivo PA imaging of cancer. In vivo experiments with 4T1 tumor-bearing mouse model demonstrated that ICG/LAP-PDA-PEG-RGD/DOX nanoplatforms exhibited much stronger therapeutic effect and higher survival rate than monotherapy due to the synergetic chemo-phototherapy under NIR laser irradiation. Therefore, the reported ICG/LAP-PDA-PEG-RGD/DOX represents a promising theranostic nanoplatform for high effectiveness PA imaging-guided chemo-phototherapy of cancer cells overexpressing αβ integrin.
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http://dx.doi.org/10.3390/nano11020394DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7913843PMC
February 2021

Facile Synthesis of Amphiphilic Fluorescent Phosphorus Dendron-Based Micelles as Antiproliferative Agents: First Investigations.

Bioconjug Chem 2021 02 31;32(2):339-349. Epub 2021 Jan 31.

Laboratoire de Chimie de Coordination du CNRS, 205 Route de Narbonne, BP 44099, 31077, Toulouse Cedex 4, France.

We designed and synthesized several families of novel amphiphilic fluorescent phosphorus dendron-based micelles showing relevant antiproliferative activities for use in the field of theranostic nanomedicine. Based on straightforward synthesis pathways, 12 amphiphilic phosphorus dendrons bearing 10 protonated cyclic amino groups (generation one), or 20 protonated amino groups (generation two), and 1 hydrophobic chain carrying 1 fluorophore moiety were created. The amphiphilic dendron micelles had the capacity to aggregate in solution using hydrophilic/hydrophobic interactions, which promoted the formation of polymeric micelles. These dendron-based micelles showed moderate to high antiproliferative activities against a panel of tumor cell lines. This paper presents for the first time the synthesis and our first investigations of new phosphorus dendron-based micelles for cancer therapy applications.
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http://dx.doi.org/10.1021/acs.bioconjchem.0c00716DOI Listing
February 2021

Antifouling Dendrimer-Entrapped Copper Sulfide Nanoparticles Enable Photoacoustic Imaging-Guided Targeted Combination Therapy of Tumors and Tumor Metastasis.

ACS Appl Mater Interfaces 2021 Feb 27;13(5):6069-6080. Epub 2021 Jan 27.

State Key Laboratory for Modification of Chemical Fiber and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

The development of functional intelligent theranostic nanoplatform for imaging-directed synchronous inhibition of primary tumor and tumor metastasis is still a challenging task. We present here the creation of functional dendrimer-entrapped CuS nanoparticles (CuS DENPs) complexed with plasmid DNA-encoding hypermethylation in cancer 1 (pDNA-HIC1) for photoacoustic (PA) imaging-directed simultaneous inhibition of tumors and tumor metastasis. Poly(amidoamine) dendrimers of generation 5 were covalently attached with 1,3-propane sultone and arginine-glycine-aspartic acid (RGD) peptide through a spacer of poly(ethylene glycol) and adopted for the templated synthesis of CuS NPs. The prepared functional RGD-CuS DENPs possess a mean CuS core diameter of 4.2 nm, good colloidal stability, and an excellent absorption feature in the second near-infrared window, thus having a photothermal conversion efficiency of 49.8% and an outstanding PA imaging capability. The functional DENPs can effectively deliver pDNA-HIC1 to prevent cancer cell invasion and metastasis in a serum-enhancing manner by virtue of zwitterionic modification-rendered antifouling property. The developed RGD-CuS DENPs/pDNA polyplexes display αβ integrin-targeted enhanced anticancer activity through the combined CuS NP-mediated photothermal therapy (PTT) and pDNA delivery-rendered cancer cell metastasis inhibition. This can also be proven by the therapeutic efficacy of a triple-negative breast cancer model , where inhibition of both the primary subcutaneous tumor and lung metastasis can be realized. The created dendrimer-CuS hybrid nanoplatform represents one of the updated designs of nanomedicine for PA imaging-directed combination PTT/gene therapy of tumors and tumor metastasis.
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http://dx.doi.org/10.1021/acsami.0c21620DOI Listing
February 2021

Synthesis and Shaping of Core-Shell Tecto Dendrimers for Biomedical Applications.

Bioconjug Chem 2021 02 18;32(2):225-233. Epub 2021 Jan 18.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, International Joint Laboratory for Advanced Fiber and Low-dimension Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

In recent years, the use of poly(amidoamine) (PAMAM) dendrimers of different generations as building blocks or reactive modules to construct core-shell tecto dendrimers (CSTDs) that are superior to the performance of single-generation dendrimers has received great attention in the field of biomedical applications. The CSTDs are always based on high-generation dendrimers as the core and low-generation dendrimers as the shell; not only do they have excellent properties similar to single high-generation dendrimers, but they also have overcome some of the shortcomings (e.g., limited drug loading capacity or enhanced permeability and retention effect due to small size) of single-generation dendrimers in biomedical applications. Herein, the recent advances of CSTDs synthesized by different approaches as nanoplatforms for different biomedical applications, particularly for chemotherapy, gene delivery, and combination therapy, as well as biological imaging, are summarized. In addition, the current challenges and future perspectives of CSTDs are also discussed.
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http://dx.doi.org/10.1021/acs.bioconjchem.1c00005DOI Listing
February 2021

Dendritic Macromolecular Architectures: Dendrimer-Based Polyion Complex Micelles.

Biomacromolecules 2021 02 11;22(2):262-274. Epub 2021 Jan 11.

Laboratoire de Chimie de Coordination du CNRS, 205 route de Narbonne, 31077, Toulouse Cedex 4, France.

Polymeric micelles are nanoassemblies that are formed by spontaneous arrangement of amphiphilic block copolymers in aqueous solutions at critical micelle concentration (CMC). They represent an effective system for drug delivery of, for instance, poorly water-soluble anticancer drugs. Then, the development of polyion complexes (PICs) were emphasized. The morphology of these complexes depends on the topology of the polyelectrolytes used and the way they are assembled. For instance, ionic-hydrophilic block copolymers have been used for the preparation of PIC micelles. The main limitation in the use of PIC micelles is their potential instability during the self-assembly/disassembly processes, influenced by several parameters, such as polyelectrolyte concentration, deionization associated with pH, ionic strength due to salt medium effects, mixing ratio, and PIC particle cross-linking. To overcome these issues, the preparation of stable PIC micelles by increasing the rigidity of their dendritic architecture by the introduction of dendrimers and controlling their number within micelle scaffold was highlighted. In this original concise Review, we will describe the preparation, molecular characteristics, and pharmacological profile of these stable nanoassemblies.
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http://dx.doi.org/10.1021/acs.biomac.0c01645DOI Listing
February 2021

Dual-mode endogenous and exogenous sensitization of tumor radiotherapy through antifouling dendrimer-entrapped gold nanoparticles.

Theranostics 2021 1;11(4):1721-1731. Epub 2021 Jan 1.

State Key Laboratory for Modification of Chemical Fiber and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

Development of a powerful sensitization system to alleviate radioresistance for enhanced tumor radiotherapy (RT) remains to be explored. Herein, we present a unique dual-mode endogenous and exogenous nanosensitizer based on dendrimer-entrapped gold nanoparticles (Au DENPs) to realize enhanced tumor RT. Generation 5 poly(amidoamine) dendrimers partially modified with 1,3-propanesultone were used for templated synthesis of Au NPs, and the created zwitterionic Au DENPs were adopted for serum-enhanced delivery of siRNA to lead to the knockdown of hypoxia-inducible factor-1α (HIF-1α) protein and downstream genes to relieve tumor invasion. The Au DENPs/siRNA polyplexes were also used for dual-mode endogenous and exogenous sensitization of tumor RT . Due to the dual-mode endogenous sensitization through HIF-1α gene silencing and the exogenous sensitization through the existing Au component, enhanced RT of cancer cells and a tumor model can be realized, which was confirmed by enhanced cytotoxic reactive oxygen species (ROS) generation and double-strand DNA damage verified from the γ-HAX protein expression in tumor cells . By integrating the advantages of HIF-1α gene silencing-induced downregulation of downstream genes and the dual-mode sensitization-enhanced RT, simultaneous inhibition of primary tumors and metastasis can be readily realized. The developed zwitterionic Au DENPs may be used as a promising platform for dual-mode endogenously and exogenously sensitized RT of other tumor types.
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http://dx.doi.org/10.7150/thno.54930DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7778585PMC
January 2021

In vivo therapeutic applications of phosphorus dendrimers: state of the art.

Drug Discov Today 2021 Mar 4;26(3):677-689. Epub 2020 Dec 4.

Laboratoire de Chimie de Coordination du CNRS, 205 route de Narbonne, 31077, Toulouse Cedex 4, France; Université Toulouse 118 route de Narbonne, 31077, Toulouse Cedex 4, France. Electronic address:

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http://dx.doi.org/10.1016/j.drudis.2020.11.034DOI Listing
March 2021

Multivalent Copper(II)-Conjugated Phosphorus Dendrimers with Noteworthy and Antitumor Activities: A Concise Overview.

Mol Pharm 2021 01 25;18(1):65-73. Epub 2020 Nov 25.

Laboratoire de Chimie de Coordination du CNRS, 205 route de Narbonne, 31077 Cedex 4 Toulouse, France.

Dendrimers are macromolecules with well-defined, homogeneous, and monodispersed structures that form a branch-like structure. In general, they have a symmetric core, inner shells, and an outer shell. Over the past decade, metallodendritic architectures have developed into a new area in nanomedicine. Due to their versatility and facile customization, phosphorus dendrimers represent interesting platforms for biomedical applications. Metallo-conjugated phosphorus dendrimers have been developed within the dendrimer space, an important part of the chemical space. The first investigation was made using phosphorus dendrimers bearing copper(II) groups on their surface as the original anticancer drug candidates. The aim of this minireview is to present our powerful strategy to find and develop original multivalent copper(II)-conjugated phosphorus dendrimers. The most potent of them is G3 dendrimers with -(pyridine-2-ylmethylene)ethanamine as the chelating motif complexed with Cu(II) (), showing very good and antiproliferative efficacy. On the basis of these results, is a potential clinical candidate having progressed from hit to preclinical candidate status.
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http://dx.doi.org/10.1021/acs.molpharmaceut.0c00892DOI Listing
January 2021

Targeted Combination of Antioxidative and Anti-Inflammatory Therapy of Rheumatoid Arthritis using Multifunctional Dendrimer-Entrapped Gold Nanoparticles as a Platform.

Small 2020 12 17;16(49):e2005661. Epub 2020 Nov 17.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, International Joint Laboratory for Advanced Fiber and Low-Dimension Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai, 201620, P. R. China.

Abundant reactive oxygen species and tumor necrosis factor-α (TNF-α) cytokine supply of M1-type macrophages boost rheumatoid arthritis (RA) pathological process. For efficient RA therapy, here a multifunctional nanoplatform is presented based on generation 5 (G5) poly(amidoamine) dendrimer-entrapped gold nanoparticles (Au DENPs) to achieve co-delivery of antioxidant alpha-tocopheryl succinate (α-TOS) and anti-inflammatory anti-TNF-α siRNA to macrophage cells. G5 dendrimers with amine termini are sequentially functionalized with 1,3-propane sultone (1,3-PS), α-TOS through a polyethylene glycol (PEG) spacer, and PEGylated folic acid (FA), and subsequently entrapped with Au NPs. The generated functional Au DENPs exhibit desired cytocompatibility, zwitterion-rendered antifouling property, and FA-mediated targeting specificity, enabling serum-enhanced siRNA delivery to M1-type macrophage cells. Meanwhile, the attached α-TOS affords enhanced oxidation resistance of macrophage cells. In vivo investigation shows that the treatment of a collagen-induced arthritis mouse model using α-TOS-modified Au DENPs/TNF-α siRNA polyplexes can achieve excellent combination therapy effect in inflammatory cytokines downregulation of RA lesion and bone erosions. The therapeutic efficacy is also supported by 3D micro-computed tomography analysis and TNF-α cytokine reduction of RA lesion joints in the mRNA, protein, and histology levels. The created multifunctional nanoplatform may be employed in antioxidative and anti-inflammatory combination therapy of RA.
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http://dx.doi.org/10.1002/smll.202005661DOI Listing
December 2020

Non-invasive intranasal administration route directly to the brain using dendrimer nanoplatforms: An opportunity to develop new CNS drugs.

Eur J Med Chem 2021 Jan 11;209:112905. Epub 2020 Oct 11.

Laboratoire de Chimie de Coordination Du CNRS, 205 Route de Narbonne, 31077, Toulouse, Cedex 4, France; Université Toulouse 118 Route de Narbonne, 31077, Toulouse, Cedex 4, France. Electronic address:

There are several routes of administration to the brain, including intraparenchymal, intraventricular, and subarachnoid injections. The blood-brain barrier (BBB) impedes the permeation and access of most drugs to the central nervous system (CNS), and consequently, many neurological diseases remain undertreated. For past decades, to circumvent this effect, several nanocarriers have been developed to deliver drugs to the brain. Importantly, intranasal (IN) administration can allow direct delivery of drugs into the brain through the anatomical connection between the nasal cavity and brain without crossing the BBB. In this regard, dendrimers may possess great potential to deliver drugs to the brain by IN administration, bypassing the BBB and reducing systemic exposure and side effects, to treat diseases of the CNS. In this original concise review, we highlighted the few examples advocated regarding the use of dendrimers to deliver CNS drugs directly via IN. This review highlighed the few examples of the association of dendrimer encapsulating drugs (e.g., small compounds: haloperidol and paeonol; macromolecular compounds: dextran, insulin and calcitonin; and siRNA) using IN administration. Good efficiencies were observed. In addition, we will present the in vivo effects of PAMAM dendrimers after IN administration, globally, showing no general toxicity.
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http://dx.doi.org/10.1016/j.ejmech.2020.112905DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7548078PMC
January 2021

Ultrasound-enhanced fluorescence imaging and chemotherapy of multidrug-resistant tumors using multifunctional dendrimer/carbon dot nanohybrids.

Bioact Mater 2021 Mar 24;6(3):729-739. Epub 2020 Sep 24.

Department of Interventional and Vascular Surgery, Shanghai Tenth People's Hospital, Tongji University School of Medicine, Shanghai, 200072, People's Republic of China.

Development of innovative nanomedicine enabling enhanced theranostics of multidrug-resistant (MDR) tumors remains to be challenging. Herein, we report the development of a newly designed multifunctional yellow-fluorescent carbon dot (y-CD)/dendrimer nanohybrids as a platform for ultrasound (US)-enhanced fluorescence imaging and chemotherapy of MDR tumors. Generation 5 (G5) poly(amidoamine) dendrimers covalently modified with efflux inhibitor of d-α-tocopheryl polyethylene glycol 1000 succinate (G5-TPGS) were complexed with one-step hydrothermally synthesized y-CDs electrostatic interaction. The formed G5-TPGS@y-CDs complexes were then physically loaded with anticancer drug doxorubicin (DOX) to generate (G5-TPGS@y-CDs)-DOX complexes. The developed nanohybrids display a high drug loading efficiency (40.7%), strong y-CD-induced fluorescence emission, and tumor microenvironment pH-preferred DOX release profile. Attributing to the DOX/TPGS dual drug design, the (G5-TPGS@y-CDs)-DOX complexes can overcome the multidrug resistance (MDR) of cancer cells and effectively inhibit the growth of cancer cells and tumors. Furthermore, the introduction of US-targeted microbubble destruction technology was proven to render the complexes with enhanced intracellular uptake and anticancer efficacy and improved chemotherapeutic efficacy and fluorescence imaging of tumors due to the produced sonoporation effect. The developed multifunctional dendrimer/CD nanohybrids may represent an advanced design of nanomedicine for US-enhanced theranostics of different types of MDR tumors.
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http://dx.doi.org/10.1016/j.bioactmat.2020.09.015DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7519212PMC
March 2021

Functional LAPONITE Nanodisks Enable Targeted Anticancer Chemotherapy .

Bioconjug Chem 2020 10 1;31(10):2404-2412. Epub 2020 Oct 1.

Department of Interventional and Vascular Surgery, Shanghai Tenth People's Hospital, Tongji University School of Medicine, Shanghai 200072, People's Republic of China.

Development of nanoplatforms for targeted anticancer drug delivery for effective tumor therapy still remains challenging in the development of nanomedicine. Here, we present a facile method to formulate a LAPONITE (LAP) nanodisk-based nanosystem for anticancer drug doxorubicin (DOX) delivery to folic acid (FA) receptor-overexpressing tumors. In the current work, aminated LAP nanodisks were first prepared through silanization, then functionalized with polyethylene glycol-linked FA (PEG-FA) via 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride (EDC) chemistry, and finally employed to physically encapsulate DOX. The formed functional LAP nanodisks (for short, LM-PEG-FA) possess a high DOX loading efficiency (88.6 ± 1.2%) and present a pH-dependent release feature with a quicker DOX release under acidic pH conditions (pH 5.0) than under physiological pH conditions (pH 7.4). flow cytometry, confocal microscopic observation, and cell viability assay show that the LM-PEG-FA/DOX complexes can be specifically taken up by FAR-overexpressing human ovarian cancer cells (SK-OV-3 cells) and present a specific cancer cell therapeutic effect. Further tumor treatment results reveal that the LM-PEG-FA/DOX complexes can exert a specific therapeutic efficacy to a xenografted SK-OV-3 tumor model when compared with nontargeted LM-PEG/DOX complexes. Therefore, the developed LM-PEG-FA nanodisks could be employed as a potential platform for targeted cancer chemotherapy.
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http://dx.doi.org/10.1021/acs.bioconjchem.0c00473DOI Listing
October 2020

Effect of Attapulgite-Doped Electrospun Fibrous PLGA Scaffold on Pro-Osteogenesis and Barrier Function in the Application of Guided Bone Regeneration.

Int J Nanomedicine 2020 11;15:6761-6777. Epub 2020 Sep 11.

Department of Oral Surgery, Shanghai Ninth People's Hospital, College of Stomatology, Shanghai Jiaotong University School of Medicine; National Clinical Research Center for Oral Diseases; Shanghai Key Laboratory of Stomatology & Shanghai Research Institute of Stomatology, Shanghai, People's Republic of China.

Purpose: Guided bone regeneration (GBR) therapy, which is a widely used technique in clinical practice and is effective in improving the repair of alveolar bone defects or bone mass deficiency regeneration, requires the use of membrane materials with good biocompatibility, barrier function, rigidity matching the space maintenance ability, economic benefits and excellent clinical applicability. The aim of this study was to develop an electrospun attapulgite (ATT)-doped poly (lactic-co-glycolic acid) (PLGA) scaffold (PLGA/ATT scaffold) as a novel material for GBR applications.

Methods And Results: Scanning electron microscopy (SEM) and X-ray diffraction (XRD) were used to determine the morphology and the crystalline structure of the PLGA/ATT scaffolds, respectively. Porosity and contact-angle measurements were also carried out to further characterize the physical properties of the PLGA/ATT scaffolds. The results of in vitro studies showed that bone marrow mesenchymal stem cells (BMSCs) attached more readily to and spread better over the PLGA/ATT scaffolds than the Bio-Gide membrane. Furthermore, in the in vitro osteoinductive experiments with BMSCs, the PLGA/ATT scaffolds were found to enhance the activity of alkaline phosphatase (ALP), promote the formation of mineralized bone nodules, and up-regulate the expression of several osteogenic markers-namely, runt-related transcription factor 2, alkaline phosphatase, osteopontin, and osteocalcin-which are similar to the effects of the Bio-Gide membrane. Further, in in vivo studies, the results of sequential fluorescent labeling, micro-computed tomography, and histological analysis suggest that using the PLGA/ATT scaffolds for repairing V-shaped buccal dehiscence on a dog's tooth root improved bone regeneration, which is not only similar to the result obtained using the Bio-Gide membrane but also much better than that obtained using PLGA scaffolds and the negative control.

Conclusion: To achieve satisfactory therapeutic results and to lower the cost of GBR treatment, this study provided a promising alternative material of bio-degradable membrane in clinical treatment.
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http://dx.doi.org/10.2147/IJN.S244533DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7494386PMC
November 2020

Colorimetric detection of Cr ions in aqueous solution using poly(γ-glutamic acid)-stabilized gold nanoparticles.

Anal Methods 2020 06;12(24):3145-3150

Department of Interventional and Vascular Surgery, Shanghai Tenth People's Hospital, Tongji University School of Medicine, Shanghai 200072, China.

Detection of heavy metal ions in water is of paramount significance for environmental pollution control. Here, we report the use of γ-polyglutamic acid (γ-PGA)-stabilized gold nanoparticles (γ-PGA-Au NPs) as a probe to sense trivalent chromium (Cr3+) in aqueous solution. In our study, γ-PGA-Au NPs were first formed through one-step sodium borohydride reduction of Au salt in the presence of γ-PGA. The formed γ-PGA-Au NPs with a mean particle size of 4.6 nm show desirable colloidal stability and a significant color change from wine red to gray after exposure to Cr3+ ions, which is visible to the naked eye and easily detected by colorimetric assay using UV-vis spectrometry. The limit of detection of Cr3+ ions is 100 ppb by the naked eye and 0.2 ppb by UV-vis spectroscopy, respectively. We further show that the detection of Cr3+ using γ-PGA-Au NPs has excellent selectivity, and the recovery percentage is higher than 82% for different water samples such as lake water, river water, tap water or mineral water. Our study demonstrates that γ-PGA-Au NPs can be utilized as an efficient probe for colorimetric sensing of Cr3+ ions in a water environment.
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http://dx.doi.org/10.1039/d0ay00842gDOI Listing
June 2020

Phosphorus dendrimers as powerful nanoplatforms for drug delivery, as fluorescent probes and for liposome interaction studies: A concise overview.

Eur J Med Chem 2020 Dec 31;208:112788. Epub 2020 Aug 31.

Laboratoire de Chimie de Coordination Du CNRS, 205 Route de Narbonne, 31077, Toulouse Cedex 4, France; Université Toulouse, 118 Route de Narbonne, 31077, Toulouse Cedex 4, France. Electronic address:

Gene therapy is a new and promising tool to treat many severe diseases and the silencing of proteins is the safest and the most efficient tool to treat diseases because it does not induce changes in human genome and avoids a huge problem encompassing insertional mutagenesis. Using small RNAs to switch on/off target proteins is limited due to existence of some barriers for them in the human body (blood RNAses, serum albumins, cell walls, etc). For therapeutic applications they need the efficient and non-toxic carrier which will deliver them into cell cytoplasm. Within the huge range of carriers available, dendrimers can be underlined as new promising efficient carriers. This review summarizes several findings in phosphorus dendrimers based on in vitro and in vivo studies. As a result, we can conclude that advantages of phosphorus dendrimers are strong interaction with siRNA/DNA and formation of small and compact positively charged complexes of high and fast penetration into cells; efficient release of siRNA/pDNA in endosomes due to "proton sponge" effect; possibility of their modification including addition of fluorescent probes - in this case fluorescent dendrimer can be used both as a gene carrier and a tracer of delivery into cells. Additional benefit of using fluorescent phosphorus dendrimers is their ability to monitor the macrophage physiological status in vitro and in vivo.
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http://dx.doi.org/10.1016/j.ejmech.2020.112788DOI Listing
December 2020

Surface-Charge-Switchable Nanoclusters for Magnetic Resonance Imaging-Guided and Glutathione Depletion-Enhanced Photodynamic Therapy.

ACS Nano 2020 09 18;14(9):11225-11237. Epub 2020 Aug 18.

Bio-Organic Chemistry, Institute for Complex Molecular Systems, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.

Photodynamic therapy (PDT) is an effective noninvasive therapeutic method that employs photosensitizers (PSs) converting oxygen to highly cytotoxic singlet oxygen (O) under light irradiation. The conventional PDT efficacy is, however, compromised by the nonspecific delivery of PSs to tumor tissue, the hypoxic tumor microenvironment, and the reduction of generated O by the intracellular antioxidant glutathione (GSH). Herein, an intelligent multifunctional synergistic nanoplatform (CMGCC) for -weighted magnetic resonance (MR) imaging-guided enhanced PDT is presented, which consists of nanoparticles composed of catalase (CAT) and manganese dioxide (MnO) that are integrated within chlorin-e6-modified glycol chitosan (GC) polymeric micelles. In this system, (1) GC polymers with pH-sensitive surface charge switchability from neutral to positive could improve the PS accumulation within the tumor region, (2) CAT could effectively reoxygenate the hypoxic tumor catalyzing endogenous hydrogen peroxide to O, and (3) MnO could consume the intracellular GSH while simultaneously producing Mn as a contrast agent for -weighted MR imaging. The CMGCC particles possess uniform size distribution, well-defined structure, favorable enzyme activity, and superior O generation ability. Both and experiments demonstrate that the CMGCC exhibit significantly enhanced PDT efficacy toward HeLa cells and subcutaneous HeLa tumors. Our study thereby demonstrates this to be a promising synergistic theranostic nanoplatform with highly efficient PDT performance for cancer therapy.
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http://dx.doi.org/10.1021/acsnano.0c03080DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7513467PMC
September 2020

Highly Doped Upconversion Nanoparticles for Applications Under Mild Excitation Power.

Anal Chem 2020 08 10;92(16):10913-10919. Epub 2020 Aug 10.

Institute for Biomedical Materials and Devices (IBMD), Faculty of Science, University of Technology Sydney, Sydney, New South Wales 2007, Australia.

One of the major challenges in using upconversion nanoparticles (UCNPs) is to improve their brightness. This is particularly true for studies, as the low power excitation is required to prevent the potential photo toxicity to live cells and tissues. Here, we report that the typical NaYF:Yb,Er nanoparticles can be highly doped, and the formula of NaYF:Yb,Er can gain orders of magnitude more brightness, which is applicable to a range of mild 980 nm excitation power densities, from 0.005 W/cm to 0.5 W/cm. Our results reveal that the concentration of Yb sensitizer ions plays an essential role, while increasing the doping concentration of Er activator ions to 6 mol % only has incremental effect. We further demonstrated a type of bright UCNPs 12 nm in total diameter for tumor imaging at a power density as low as 0.0027 W/cm, bringing down the excitation power requirement by 42 times. This work redefines the doping concentrations to fight for the issue of concentration quenching, so that ultrasmall and bright nanoparticles can be used to further improve the performance of upconversion nanotechnology in photodynamic therapy, light-triggered drug release, optogenetics, and night vision enhancement.
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http://dx.doi.org/10.1021/acs.analchem.0c02143DOI Listing
August 2020

Dendrimers toward Translational Nanotherapeutics: Concise Key Step Analysis.

Bioconjug Chem 2020 09 26;31(9):2060-2071. Epub 2020 Aug 26.

Laboratoire de Chimie de Coordination du CNRS, 205 route de Narbonne, 31077, Toulouse, Cedex 4, France.

The goal of nanomedicine is to address specific clinical problems optimally, to fight human diseases, and to find clinical relevance to change clinical practice. Nanomedicine is poised to revolutionize medicine via the development of more precise diagnostic and therapeutic tools. The field of nanomedicine encompasses numerous features and therapeutic disciplines. A plethora of nanomolecular structures have been engineered and developed for therapeutic applications based on their multitasking abilities and the wide functionalization of their core scaffolds and surface groups. Within nanoparticles used for nanomedicine, dendrimers as well polymers have demonstrated strong potential as nanocarriers, therapeutic agents, and imaging contrast agents. In this review, we present and discuss the different criteria and parameters to be addressed to prepare and develop druggable nanoparticles in general and dendrimers in particular. We also describe the major requirements, included in the preclinical and clinical roadmap, for NPs/dendrimers for the preclinical stage to commercialization. Ultimately, we raise the clinical translation of new nanomedicine issues.
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http://dx.doi.org/10.1021/acs.bioconjchem.0c00395DOI Listing
September 2020

Hybrid nanogels with unique designs for improved tumor theranostics.

Nanomedicine (Lond) 2020 06 9;15(15):1455-1458. Epub 2020 Jun 9.

State Key Laboratory for Modification of Chemical Fibers & Polymer Materials, International Joint Laboratory for Advanced Fiber & Low-dimension Materials, College of Chemistry, Chemical Engineering & Biotechnology, Donghua University, Shanghai, 201620, PR China.

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http://dx.doi.org/10.2217/nnm-2020-0142DOI Listing
June 2020

Adoptive cellular immunotherapy of tumors via effective CpG delivery to dendritic cells using dendrimer-entrapped gold nanoparticles as a gene vector.

J Mater Chem B 2020 06 13;8(23):5052-5063. Epub 2020 May 13.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

The major obstacle that hinders current cancer immunotherapies is the development of an effective approach to promote a proper immune response for effective tumor killing through activated T cells. Herein, we report an effective T cell-based tumor immunotherapy approach through nonviral delivery of a cytosine-guanine (CpG) oligonucleotide using dendrimer-entrapped gold nanoparticles (Au DENPs). In our work, Au DENPs partially decorated with methoxy polyethylene glycol (mPEG) were synthesized and characterized to be used as a vector for CpG delivery to bone marrow-derived dendritic cells (BMDCs). The BMDCs matured via CpG delivery were used to activate T cells for adoptive immunotherapy of cancer cells. We show that the developed PEGylated Au DENPs are able to effectively transfect CpG leading to the maturation of BMDCs that can be used to activate T cells for subsequent adoptive immunotherapy of cancer cells in vitro and a xenografted melanoma tumor model in vivo after intravenous injection. Importantly, the developed approach to genetically engineer BMDCs enables a triggered adaptive immune response and memory of T cells, which can be beneficial for effective inhibition of tumor metastasis and recurrence. The developed nonviral gene delivery approach using Au DENPs as a vector for T cell-based immunotherapy can be applied to different cancer types.
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http://dx.doi.org/10.1039/d0tb00678eDOI Listing
June 2020

Revisiting Cationic Phosphorus Dendrimers as a Nonviral Vector for Optimized Gene Delivery Toward Cancer Therapy Applications.

Biomacromolecules 2020 06 11;21(6):2502-2511. Epub 2020 May 11.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

Gene delivery, one important cancer-therapy mode, still remains to be challenging because of the shortage of highly efficient and safe nonviral vectors. Here, we revisit the development of cationic phosphorus dendrimers by synthesizing them with different generations (G1-3) and surface ligands (1-(2-aminoethyl) pyrrolidine, 1-(3-aminopropyl) piperidine, or 1-(2-aminoethyl) piperidine) for optimized gene delivery toward cancer-gene-therapy applications. First, the synthesized dendrimer derivatives were employed to condense plasmid DNA (pDNA) encoding enhanced green fluorescent protein (EGFP) to optimize their gene-delivery efficiency by varying the dendrimer generations and surface polycationic ligands. We show that all dendrimer/pDNA polyplexes display good cytocompatibility, and the 1-(2-aminoethyl) pyrrolidine-modified protonated G1 dendrimers (1-G1) display the best gene-delivery efficiency to HeLa cells under the same conditions through flow cytometry and fluorescence microscopic imaging analyses. Hence, 1-G1 dendrimers were then used as a vector to transfect pDNA encoding both EGFP and p53 protein for cancer-gene-therapy applications. Our results reveal that under the optimized conditions, the transfection of pDNA induces the significant p53 protein expression as verified through the resulted cell cycle arrest (regulation of p21 and Cdk4/Cyclin-D1 expression) and Western blotting. The cancer-gene-therapy potential of the polyplexes was finally validated through therapy of a xenografted tumor model after intratumoral injection without systemic toxicity. The developed cationic 1-G1 dendrimers may be adopted as a powerful vector system for gene therapy of cancer, as well as for highly effective gene therapy of other diseases.
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http://dx.doi.org/10.1021/acs.biomac.0c00458DOI Listing
June 2020

Multifunctional PVCL nanogels with redox-responsiveness enable enhanced MR imaging and ultrasound-promoted tumor chemotherapy.

Theranostics 2020 15;10(10):4349-4358. Epub 2020 Mar 15.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, International Joint Laboratory for Advanced Fiber and Low-dimension Materials, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, People's Republic of China.

Development of versatile nanoplatforms that simultaneously integrate therapeutic and diagnostic features for stimuli-responsive delivery to tumors remains a great challenge. In this work, we report a novel intelligent redox-responsive hybrid nanosystem composed of MnO nanoparticles (NPs) and doxorubicin (DOX) co-loaded within poly(N-vinylcaprolactam) nanogels (PVCL NGs) for magnetic resonance (MR) imaging-guided and ultrasound-targeted microbubble destruction (UTMD)-promoted tumor chemotherapy. : PVCL NGs were first synthesized a precipitation polymerization method, decorated with amines using ethylenediamine, and loaded with MnO NPs through oxidation with permanganate and DOX physical encapsulation and Mn-N coordination bonding. The as-prepared DOX/MnO@PVCL NGs were well characterized. UTMD-promoted cellular uptake and therapeutic efficacy of the hybrid NGs were assessed , and a xenografted tumor model was used to test the NGs for MR imaging and UTMD-promoted tumor therapy : The as-prepared DOX/MnO@PVCL NGs with a size of 106.8 nm display excellent colloidal stability, favorable biocompatibility, and redox-responsiveness to the reductive intracellular environment and tumor tissues having a relatively high glutathione (GSH) concentration that can trigger the synchronous release of Mn for enhanced T-weighted MR imaging and DOX for enhanced cancer chemotherapy. Moreover, the DOX/MnO@PVCL NGs upon the UTMD-promotion exhibit a significantly enhanced tumor growth inhibition effect toward subcutaneous B16 melanoma owing to the UTMD-improved cellular internalization and tumor penetration. : Our work thereby proposes a promising theranostic nanoplatform for stimuli-responsive T-weighted MR imaging-guided tumor chemotherapy.
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http://dx.doi.org/10.7150/thno.43402DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7150492PMC
April 2021