Publications by authors named "Chong Cheng"

120 Publications

Designing MOF Nanoarchitectures for Electrochemical Water Splitting.

Adv Mater 2021 Mar 22:e2006042. Epub 2021 Mar 22.

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, 610065, China.

Electrochemical water splitting has attracted significant attention as a key pathway for the development of renewable energy systems. Fabricating efficient electrocatalysts for these processes is intensely desired to reduce their overpotentials and facilitate practical applications. Recently, metal-organic framework (MOF) nanoarchitectures featuring ultrahigh surface areas, tunable nanostructures, and excellent porosities have emerged as promising materials for the development of highly active catalysts for electrochemical water splitting. Herein, the most pivotal advances in recent research on engineering MOF nanoarchitectures for efficient electrochemical water splitting are presented. First, the design of catalytic centers for MOF-based/derived electrocatalysts is summarized and compared from the aspects of chemical composition optimization and structural functionalization at the atomic and molecular levels. Subsequently, the fast-growing breakthroughs in catalytic activities, identification of highly active sites, and fundamental mechanisms are thoroughly discussed. Finally, a comprehensive commentary on the current primary challenges and future perspectives in water splitting and its commercialization for hydrogen production is provided. Hereby, new insights into the synthetic principles and electrocatalysis for designing MOF nanoarchitectures for the practical utilization of water splitting are offered, thus further promoting their future prosperity for a wide range of applications.
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http://dx.doi.org/10.1002/adma.202006042DOI Listing
March 2021

Valorisation of medical waste through pyrolysis for a cleaner environment: Progress and challenges.

Environ Pollut 2021 Mar 11;279:116934. Epub 2021 Mar 11.

China-UK Low Carbon College, Shanghai Jiao Tong University, Lingang, Shanghai, 201306, China.

The COVID-19 pandemic has exerted great shocks and challenges to the environment, society and economy. Simultaneously, an intractable issue appeared: a considerable number of hazardous medical wastes have been generated from the hospitals, clinics, and other health care facilities, constituting a serious threat to public health and environmental sustainability without proper management. Traditional disposal methods like incineration, landfill and autoclaving are unable to reduce environmental burden due to the issues such as toxic gas release, large land occupation, and unsustainability. While the application of clean and safe pyrolysis technology on the medical wastes treatment to produce high-grade bioproducts has the potential to alleviate the situation. Besides, medical wastes are excellent and ideal raw materials, which possess high hydrogen, carbon content and heating value. Consequently, pyrolysis of medical wastes can deal with wastes and generate valuable products like bio-oil and biochar. Consequently, this paper presents a critical and comprehensive review of the pyrolysis of medical wastes. It demonstrates the feasibility of pyrolysis, which mainly includes pyrolysis characteristics, product properties, related problems, the prospects and future challenges of pyrolysis of medical wastes.
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http://dx.doi.org/10.1016/j.envpol.2021.116934DOI Listing
March 2021

Heteromultivalent topology-matched nanostructures as potent and broad-spectrum influenza A virus inhibitors.

Sci Adv 2021 01 1;7(1). Epub 2021 Jan 1.

Institut für Chemie und Biochemie Organische Chemie, Freie Universität Berlin, Takustr. 3, 14195 Berlin, Germany.

Here, we report the topology-matched design of heteromultivalent nanostructures as potent and broad-spectrum virus entry inhibitors based on the host cell membrane. Initially, we investigate the virus binding dynamics to validate the better binding performance of the heteromultivalent moieties as compared to homomultivalent ones. The heteromultivalent binding moieties are transferred to nanostructures with a bowl-like shape matching the viral spherical surface. Unlike the conventional homomultivalent inhibitors, the heteromultivalent ones exhibit a half maximal inhibitory concentration of 32.4 ± 13.7 μg/ml due to the synergistic multivalent effects and the topology-matched shape. At a dose without causing cellular toxicity, >99.99% reduction of virus propagation has been achieved. Since multiple binding sites have also been identified on the S protein of SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2), we envision that the use of heteromultivalent nanostructures may also be applied to develop a potent inhibitor to prevent coronavirus infection.
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http://dx.doi.org/10.1126/sciadv.abd3803DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7775783PMC
January 2021

Fast photocurable thiol-ene elastomers with tunable biodegradability, mechanical and surface properties enhance myoblast differentiation and contractile function.

Bioact Mater 2021 Jul 12;6(7):2120-2133. Epub 2021 Jan 12.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.

Biodegradable elastomers are important emerging biomaterials for biomedical applications, particularly in the area of soft-tissue engineering in which scaffolds need to match the physicochemical properties of native tissues. Here, we report novel fast photocurable elastomers with readily tunable mechanical properties, surface wettability, and degradability. These elastomers are prepared by a 5-min UV-irradiation of thiol-ene reaction systems of glycerol tripentenoate (GTP; a triene) or the combination of GTP and 4-pentenyl 4-pentenoate (PP; a diene) with a carefully chosen series of di- or tri-thiols. In the subsequent application study, these elastomers were found to be capable of overcoming delamination of myotubes, a technical bottleneck limiting the growth of mature functional myofibers. The glycerol-based elastomers supported the proliferation of mouse and human myoblasts, as well as myogenic differentiation into contractile myotubes. More notably, while beating mouse myotubes detached from conventional tissue culture plates, they remain adherent on the elastomer surface. The results suggest that these elastomers as novel biomaterials may provide a promising platform for engineering functional soft tissues with potential applications in regenerative medicine or pharmacological testing.
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http://dx.doi.org/10.1016/j.bioactmat.2020.12.022DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7810627PMC
July 2021

The COVID-19 pandemic face mask waste: A blooming threat to the marine environment.

Chemosphere 2021 Jun 9;272:129601. Epub 2021 Jan 9.

Center of Excellence in Catalysis for Bioenergy and Renewable Chemicals (CBRC), Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand; Center of Excellence on Petrochemical and Materials Technology (PETROMAT), Chulalongkorn University, Pathumwan, Bangkok 10330, Thailand. Electronic address:

Recently, the COVID-19 disease spread has emerged as a worldwide pandemic and cause severe threats to humanity. The World Health Organisation (WHO) releases guidelines to help the countries to reduce the spread of this virus to the public, like wearing masks, hand hygiene, social distancing, shutting down all types of public transports, etc. These conditions led to a worldwide economic fall drastically, and on the other hand, indirect environmental benefits like global air quality improvement and decreased water pollution are also pictured. Currently, use of face masks is part of a comprehensive package of the prevention and control measures that can limit the spread of COVID-19 since there is no clinically proven drugs or vaccine available for COVID-19. Mostly, face masks are made of petroleum-based non-renewable polymers that are non-biodegradable, hazardous to the environment and create health issues. This study demonstrates the extensive use of the face mask and how it affects human health and the marine ecosystem. It has become a great challenge for the government sectors to impose strict regulations for the proper disposal of the masks as medical waste by the public. Neglecting the seriousness of this issue may lead to the release of large tonnes of micro-plastics to the landfill as well as to the marine environment where mostly end-up and thereby affecting their fauna and flora population vastly. Besides, this study highlights the COVID-19 spread, its evolutionary importance, taxonomy, genomic structure, transmission to humans, prevention, and treatment.
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http://dx.doi.org/10.1016/j.chemosphere.2021.129601DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7836388PMC
June 2021

Bioinspired Spiky Peroxidase-Mimics for Localized Bacterial Capture and Synergistic Catalytic Sterilization.

Adv Mater 2021 Feb 21;33(8):e2005477. Epub 2021 Jan 21.

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Department of Ultrasound, West China Hospital, Sichuan University, Chengdu, 610065, China.

Besides the pandemic caused by the coronavirus outbreak, many other pathogenic microbes also pose a devastating threat to human health, for instance, pathogenic bacteria. Due to the lack of broad-spectrum antibiotics, it is urgent to develop nonantibiotic strategies to fight bacteria. Herein, inspired by the localized "capture and killing" action of bacteriophages, a virus-like peroxidase-mimic (V-POD-M) is synthesized for efficient bacterial capture (mesoporous spiky structures) and synergistic catalytic sterilization (metal-organic-framework-derived catalytic core). Experimental and theoretical calculations show that the active compound, MoO , can serve as a peroxo-complex-intermediate to reduce the free energy for catalyzing H O , which mainly benefits the generation of •OH radicals. The unique virus-like spikes endow the V-POD-M with fast bacterial capture and killing abilities (nearly 100% at 16 µg mL ). Furthermore, the in vivo experiments show that V-POD-M possesses similar disinfection treatment and wound skin recovery efficiencies to vancomycin. It is suggested that this inexpensive, durable, and highly reactive oxygen species (ROS) catalytic active V-POD-M provides a promising broad-spectrum therapy for nonantibiotic disinfection.
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http://dx.doi.org/10.1002/adma.202005477DOI Listing
February 2021

Synthesis and antibacterial activity of polymer-antibiotic conjugates incorporated into a resin-based dental adhesive.

Biomater Sci 2021 Mar 19;9(6):2043-2052. Epub 2021 Jan 19.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, USA.

This work reports on polymer-antibiotic conjugates (PACs) as additives to resin-based restorative dental materials as a new strategy to convey sustained antibacterial character to these materials. Such antibacterial performance is expected to improve their longevity in the oral cavity. Using the previously reported ciprofloxacin (Cip)-based PAC as a control, a penicillin V (PV)-based PAC was investigated. The monomer-antibiotic conjugate (MAC) containing a methacrylate monomer group and a PV moiety was prepared via nucleophilic substitution between 2-chloroethyl methacrylate (CEMA) and penicillin V potassium (PVK). The PV-based PAC was synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization of the MAC with hydroxyethyl methacrylate (HEMA), and further characterized by H NMR and gel permeation chromatography (GPC) analysis. Antibiotic resistance was investigated by passaging bacteria in low concentrations of the antibiotic for 19 days, followed by a 48 h challenge at higher concentrations. Our results suggest that the development of antibiotic resistance is unlikely. Zone of inhibition (ZOI) assays revealed no clearing zones around PV-containing resins indicating minimal antibiotic leakage from the material. Similarly, MTT assay demonstrated that the antibiotic-containing specimens did not release cytotoxic byproducts that may inhibit human gingival fibroblast growth. Counting of colony-forming units in an S. mutans biofilm model was used to assess bacterial survival at baseline and after subjecting the antibiotic-containing resin specimens to an enzymatic challenge for 30 days. Significantly reduced bacterial counts were observed as the biofilm aged from 24 to 72 h, and salivary enzymatic exposure did not reduce the antibacterial efficacy of the discs, suggesting that PV-resin will be effective in reducing the re-incidence of dental caries.
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http://dx.doi.org/10.1039/d0bm01910kDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7990707PMC
March 2021

Spiky nanostructures for virus inhibition and infection prevention.

Smart Mater Med 2020 16;1:48-53. Epub 2020 Jul 16.

College of Polymer Science and Engineering, Sichuan University, No.24 South Section 1, Yihuan Road, Chengdu, 610065, China.

The outbreak of a novel highly infectious virus, severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), has aroused people's concern about public health. The lack of ready-to-use vaccines and therapeutics makes the fight with these pathogens extremely difficult. To this point, rationally designed virus entry inhibitors that block the viral interaction with its receptor can be novel strategies to prevent virus infection. For ideal inhibition of the virus, the virus-inhibitor interaction has to outperform the virus-host interaction. In our view, the morphology of the inhibitor should be carefully designed to benefit virus-inhibitor binding, especially that the surfaces of viruses are mostly rough due to the existence of surface proteins for receptor-binding. In this perspective article, we would like to discuss the recent progress of designing inhibitors with spiky topography to maximize the interactions between viruses and inhibitors. We also would like to share our idea for the future study of inhibitors to prevent virus infection.
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http://dx.doi.org/10.1016/j.smaim.2020.07.004DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7363616PMC
July 2020

Transition Metal and Metal-N Codoped MOF-Derived Fenton-Like Catalysts: A Comparative Study on Single Atoms and Nanoparticles.

Small 2020 12 23;16(50):e2005060. Epub 2020 Nov 23.

College of Biomass Science and Engineering, College of Polymer Science and Engineering, West China School of Medicine/West China Hospital, Sichuan University, Chengdu, 610065, China.

To deal with the ever-growing toxic benzene-derived compounds in the water system, extensive efforts have been dedicated for catalytic degradation of pollutants. However, the activities and efficiencies of the transition metal-based nanoparticles or single-atom sites are still ambiguous in Fenton-like reactions. Herein, to compare the Fenton-like catalytic efficiencies of the nanoparticles and single atoms, the free-standing nanofibrous catalyst comprising Co nanocrystals and Co-N codoped carbon nanotubes (CNTs) or bare Co-N doped CNTs is fabricated. It is noteworthy that all these nanofibrous catalysts exhibit efficient activities, mesoporous structures, and conductive carbon networks, which allow a feasible validation of the catalytic effects. Benefiting from the maximized atomic utilization, the atomic Co-N centers exhibit much higher reaction kinetic constant (κ = 0.157 min ) and mass activity toward the degradation of bisphenol A, far exceeding the Co nanocrystals (κ = 0.082 min ). However, for the volume activities, the single-atom catalyst does not show apparent advantages compared to the nanocrystal-based catalyst. Overall, this work not only provides a viable pathway for comparing Fenton-like catalytic effects of transition metal-based nanoparticles or single atoms but also opens up a new avenue for developing prominent catalysts for organic pollutants' degradation.
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http://dx.doi.org/10.1002/smll.202005060DOI Listing
December 2020

Kaempferol promotes BMSC osteogenic differentiation and improves osteoporosis by downregulating miR-10a-3p and upregulating CXCL12.

Mol Cell Endocrinol 2021 01 3;520:111074. Epub 2020 Nov 3.

Department of Rehabilitation, The Second Affiliated Hospital of Nanchang University, Nanchang, 330006, China. Electronic address:

Background: Kaempferol has improved the functions of various human diseases. Here, we aimed to probe into the potential molecular mechanism of Kaempferol to ameliorate osteoporosis.

Methods: Micro-computed tomography scanning was applied to assess the bone density of osteoporosis rats induced by ovariectomized. Quantitative real-time PCR was applied to detect the expressions of RUNX2, Osterix, CXCL12, and miR-10a-3p. Western blot, Alizarin red staining, Alkaline Phosphatase Diethanolamine Activity Kit were applied to confirm the in vitro functions of Kaempferol. RNA Immunoprecipitation and dual-luciferase reporter gene experiments were applied to study the potential mechanism.

Results: The treatment of Kaempferol raised bone density in osteoporosis rats induced by ovariectomized, and boosted the osteogenic differentiation of bone marrow mesenchymal stem cells (BMSCs), and raised the expressions of RUNX2, Osterix, and CXCL12, and lessened miR-10a-3p. From the potential mechanism analysis, we corroborated that miR-10a-3p and CXCL12 bound to each other, and Kaempferol boosted BMSC osteogenic differentiation and ameliorated osteoporosis by lessening miR-10a-3p and raising CXCL12.

Conclusion: Our data expounded that Kaempferol boosted BMSC osteogenic differentiation and ameliorated osteoporosis by lessening miR-10a-3p and raising CXCL12.
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http://dx.doi.org/10.1016/j.mce.2020.111074DOI Listing
January 2021

Metal-Organic-Framework-Engineered Enzyme-Mimetic Catalysts.

Adv Mater 2020 Dec 30;32(49):e2003065. Epub 2020 Oct 30.

Department of Ultrasound, West China Hospital, College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, 610065, China.

Nanomaterial-based enzyme-mimetic catalysts (Enz-Cats) have received considerable attention because of their optimized and enhanced catalytic performances and selectivities in diverse physiological environments compared with natural enzymes. Recently, owing to their molecular/atomic-level catalytic centers, high porosity, large surface area, high loading capacity, and homogeneous structure, metal-organic frameworks (MOFs) have emerged as one of the most promising materials in engineering Enz-Cats. Here, the recent advances in the design of MOF-engineered Enz-Cats, including their preparation methods, composite constructions, structural characterizations, and biomedical applications, are highlighted and commented upon. In particular, the performance, selectivities, essential mechanisms, and potential structure-property relations of these MOF-engineered Enz-Cats in accelerating catalytic reactions are discussed. Some potential biomedical applications of these MOF-engineered Enz-Cats are also breifly proposed. These applications include, for example, tumor therapies, bacterial disinfection, tissue regeneration, and biosensors. Finally, the future opportunities and challenges in emerging research frontiers are thoroughly discussed. Thereby, potential pathways and perspectives for designing future state-of-the-art Enz-Cats in biomedical sciences are offered.
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http://dx.doi.org/10.1002/adma.202003065DOI Listing
December 2020

Maximizing the grafting of zwitterions onto the surface of ultrafiltration membranes to improve antifouling properties.

J Memb Sci 2020 ;601

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.

Superhydrophilic zwitterions have been extensively exploited for surface modification to improve antifouling properties. However, it remains challenging to form layers of < 20 nm with high zwitterion content on the surfaces with different degrees of hydrophilicity. We demonstrate that amine-functionalized sulfobetaine (SBAm) can be co-deposited with dopamine on ultrafiltration (UF) membranes, leading to a thickness of 10 nm to 50 nm and an SBAm content of up to 31 mass% in the coating layers. The covalently grafted SBAm is stable underwater and improves the antifouling properties, as evidenced by the lower trans-membrane pressure required to retain targeted water fluxes than that required for the pristine membranes. The SBAm is also more effective than conventionally used sulfobetaine methacrylate (SBMA) for the zwitterion grafting on the surface to improve antifouling properties.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7539668PMC
January 2020

Biocompatibility, mechanical, and bonding properties of a dental adhesive modified with antibacterial monomer and cross-linker.

Clin Oral Investig 2020 Oct 2. Epub 2020 Oct 2.

Department of Restorative Dentistry, School of Dental Medicine, University at Buffalo, 215 Squire Hall, 3435 Main Street, Buffalo, NY, 14214, USA.

Objectives: This study investigated the antibacterial, cytotoxicity, and mechanical properties of a dental adhesive modified with quaternary ammonium monomer ((2-acryloyloxyethyl)dimethyldodecylammonium bromide) and cross-linker (bis(2-acryloyloxyethyl)methyldodecylammonium bromide).

Materials And Methods: Monomer (M), cross-linker (C), or a combination of these (M + C) were incorporated into adhesive Adper Single Bond Plus (SB) in 5, 10, or 25% (as wt%). A colony-forming unit and MTT assays were used to evaluate antibacterial properties against Streptococcus mutans and cell viability. Resin-dentin beams (0.9 ± 0.1 mm) were evaluated for micro-tensile bond strength (μTBS) after 24 h, 6 months, and 3 years. Hourglass specimens were evaluated for ultimate tensile strength (UTS) after 24 h, 1 week, and 6 months. Micro-hardness measurements after softening in ethanol were taken as an indirect assessment of the polymer cross-linking density. Kruskal-Wallis, one-way ANOVA, two-way ANOVA, and Student's t test were used for analysis of the antibacterial, cytotoxicity, μTBS, UTS, and hardness data, all with a significance level of p < 0.05.

Results: 10%M and 25%M demonstrated a significant reduction in S. mutans relative to SB (p < 0.001). No differences in cytotoxicity were detected for any of the groups. After 6 months, no changes in μTBS were shown for any of the groups. After 3 years, all groups evidenced a significant decrease in μTBS (p < 0.05) except 5%M, 5%C, and 5%M + 5%C. All groups demonstrated either stable or significantly increased UTS after 6 months. Except for the cross-linker groups, a significant decrease in micro-hardness was shown for all groups after softening in ethanol (p < 0.05).

Conclusions: A 5-10% of monomer may render the resin antibacterial without a compromise to its mechanical and bonding properties.

Clinical Relevance: Biomodification of a resin adhesive with an antibacterial monomer and cross-linker may help improve the life span of adhesive restorations.
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http://dx.doi.org/10.1007/s00784-020-03605-wDOI Listing
October 2020

Reverse design of an influenza neutralizing spiky nano-inhibitor with a dual mode of action.

Angew Chem Weinheim Bergstr Ger 2020 May 18. Epub 2020 May 18.

Freie Universitat Berlin Dept. of Biology, Chemistry and Pharmacy Takustr. 3 Institute for Chemistry and Biochemistry 14195 Berlin GERMANY.

In this study, we demonstrate the concept of 'reverse design' for virus inhibitors. With the current knowledge of influenza A virus (IAV), we designed a nano-inhibitor that has a reverse shape to the viral particle and heteromultivalent inhibitory effects on hemagglutinin and neuraminidase. The synthesized nano-inhibitor can neutralize the viral particle extracellularly and block its attachment and entry to the host cells. The virus replication was significantly reduced by 6 orders of magnitude in the presence of the reverse designed nano-inhibitors. Even being used 24 hours after the infection, >99.999% inhibition is also achieved, which indicates such a nano-inhibitor might be a potent antiviral for the treatment of influenza infection.
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http://dx.doi.org/10.1002/ange.202004832DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7276915PMC
May 2020

ZnO/Nanocarbons-Modified Fibrous Scaffolds for Stem Cell-Based Osteogenic Differentiation.

Small 2020 09 19;16(38):e2003010. Epub 2020 Aug 19.

Department of Chemistry and Biochemistry, Freie Universität Berlin, Takustrasse 3, Berlin, 14195, Germany.

Currently, mesenchymal stem cells (MSCs)-based therapies for bone regeneration and treatments have gained significant attention in clinical research. Though many chemical and physical cues which influence the osteogenic differentiation of MSCs have been explored, scaffolds combining the benefits of Zn ions and unique nanostructures may become an ideal interface to enhance osteogenic and anti-infective capabilities simultaneously. In this work, motivated by the enormous advantages of Zn-based metal-organic framework-derived nanocarbons, C-ZnO nanocarbons-modified fibrous scaffolds for stem cell-based osteogenic differentiation are constructed. The modified scaffolds show enhanced expression of alkaline phosphatase, bone sialoprotein, vinculin, and a larger cell spreading area. Meanwhile, the caging of ZnO nanoparticles can allow the slow release of Zn ions, which not only activate various signaling pathways to guide osteogenic differentiation but also prevent the potential bacterial infection of implantable scaffolds. Overall, this study may provide new insight for designing stem cell-based nanostructured fibrous scaffolds with simultaneously enhanced osteogenic and anti-infective capabilities.
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http://dx.doi.org/10.1002/smll.202003010DOI Listing
September 2020

Crosslinked polymer nanocapsules for therapeutic, diagnostic, and theranostic applications.

Wiley Interdiscip Rev Nanomed Nanobiotechnol 2020 11 3;12(6):e1653. Epub 2020 Jul 3.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA.

Crosslinked polymer nanocapsules (CPNCs) are hollowed nanoparticles with network-like polymeric shells stabilized by primary bonds. CPNCs have drawn broad and significant interests as nanocarriers for biomedical applications in recent years. As compared with conventional polymeric nanoparticles systems without cavity and/or crosslinking architectures, CPNCs possess significant biomedical relevant advantages, including (a) superior structural stability against environmental conditions, (b) high loading capacity and ability for region-specific loading of multiple cargos, (c) tuneable cargo release rate via crosslinking density, and (d) high specific surface area to facilitate surface adsorption, modification, and interactions. With appropriate base polymers and crosslinkages, CPNCs can be biocompatible and biodegradable. While CPNC-based biomedical nanoplatforms can possess relatively stable physicochemical properties owing to their crosslinked architectures, various biomedically relevant stimuli-responsivities can be incorporated with them through specific structural designs. CPNCs have been studied for the delivery of small molecule drugs, genes, proteins, and other therapeutic agents. They have also been investigated as diagnostic platforms for magnetic resonance imaging, ultrasound imaging, and optical imaging. Moreover, CPNCs have been utilized to carry both therapeutics and bioimaging agents for theranostic applications. This article reviews the therapeutic, diagnostic and theranostic applications of CPNCs, as well as the preparation of these CPNCs, reported in the past decade. This article is categorized under: Therapeutic Approaches and Drug Discovery > Nanomedicine for Oncologic Disease Implantable Materials and Surgical Technologies > Nanomaterials and Implants Diagnostic Tools > in vivo Nanodiagnostics and Imaging.
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http://dx.doi.org/10.1002/wnan.1653DOI Listing
November 2020

Ligand Diffusion Enables Force-Independent Cell Adhesion via Activating α5β1 Integrin and Initiating Rac and RhoA Signaling.

Adv Mater 2020 Jul 14;32(29):e2002566. Epub 2020 Jun 14.

Institute of Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, Berlin, 14195, Germany.

Cells reside in a dynamic microenvironment in which adhesive ligand availability, density, and diffusivity are key factors regulating cellular behavior. Here, the cellular response to integrin-binding ligand dynamics by directly controlling ligand diffusivity via tunable ligand-surface interactions is investigated. Interestingly, cell spread on the surfaces with fast ligand diffusion is independent of myosin-based force generation. Fast ligand diffusion enhances α5β1 but not αvβ3 integrin activation and initiates Rac and RhoA but not ROCK signaling, resulting in lamellipodium-based fast cell spreading. Meanwhile, on surfaces with immobile ligands, αvβ3 and α5β1 integrins synergistically initiate intracellular-force-based canonical mechanotransduction pathways to enhance cell adhesion and osteogenic differentiation of stem cells. These results indicate the presence of heretofore-unrecognized pathways, distinct from canonical actomyosin-driven mechanisms, that are capable of promoting cell adhesion.
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http://dx.doi.org/10.1002/adma.202002566DOI Listing
July 2020

Spiky Nanostructures with Geometry-matching Topography for Virus Inhibition.

Nano Lett 2020 07 9;20(7):5367-5375. Epub 2020 Jun 9.

Institut für Chemie und Biochemie Organische Chemie, Freie Universität Berlin, Takustr. 3, 14195 Berlin, Germany.

Geometry-matching has been known to benefit the formation of stable biological interactions in natural systems. Herein, we report that the spiky nanostructures with matched topography to the influenza A virus (IAV) virions could be used to design next-generation advanced virus inhibitors. We demonstrated that nanostructures with spikes between 5 and 10 nm bind significantly better to virions than smooth nanoparticles, due to the short spikes inserting into the gaps of glycoproteins of the IAV virion. Furthermore, an erythrocyte membrane (EM) was coated to target the IAV, and the obtained EM-coated nanostructures could efficiently prevent IAV virion binding to the cells and inhibit subsequent infection. In a postinfection study, the EM-coated nanostructures reduced >99.9% virus replication at the cellular nontoxic dosage. We predict that such a combination of geometry-matching topography and cellular membrane coating will also push forward the development of nanoinhibitors for other virus strains, including SARS-CoV-2.
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http://dx.doi.org/10.1021/acs.nanolett.0c01723DOI Listing
July 2020

Ultrasound-targeted microbubble destruction augmented synergistic therapy of rheumatoid arthritis via targeted liposomes.

J Mater Chem B 2020 06;8(24):5245-5256

Department of Medical Ultrasound, Laboratory of Ultrasound Imaging Drug, West China Hospital, Sichuan University, Chengdu 610041, China.

Rheumatoid arthritis (RA) can lead to joint destruction and deformity, which is a significant cause of the loss of the young and middle-aged labor force. However, the treatment of RA is still filled with challenges. Though dexamethasone, one of the glucocorticoids, is commonly used in the treatment of RA, its clinical use is limited because of the required high-dose and long-term use, unsatisfactory therapeutic effects, and various side-effects. Ultrasound-targeted microbubble destruction (UTMD) can augment the ultrasonic cavitation effects and trigger drug release from targeted nanocarriers in the synovial cavity, which makes it a more effective synergistic treatment strategy for RA. In this work, we aim to utilize the UTMD effect to augment the synergistic therapy of RA by using polyethylene glycol (PEG)-modified folate (FA)-conjugated liposomes (LPs) loaded with dexamethasone sodium phosphate (DexSP) (DexSP@LPs-PEG-FA). The UTMD-mediated DexSP@LPs-PEG-FA for targeted delivery of DexSP including a synergistic ultrasonic cavitation effect and drug therapy were investigated through in vitro RAW264.7 cell experiments and in vivo collagen-induced arthritis SD rat model animal experiments. The results show the DexSP release from targeted liposomes was improved under the UTMD effect. Likewise, the folate-conjugated liposomes displayed targeting association to RAW264.7 cells. Together with the application of ultrasound and microbubbles, liposomes-delivered DexSP potently reduced joints swelling, bone erosion, and inflammation in both joints and serum with a low dose. These results demonstrated that UTMD-mediated folate-conjugated liposomes are not only a promising method for targeted synergistic treatment of RA but also may show high potential for serving as nanomedicines for many other biomedical fields.
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http://dx.doi.org/10.1039/d0tb00430hDOI Listing
June 2020

Topology-Matching Design of an Influenza-Neutralizing Spiky Nanoparticle-Based Inhibitor with a Dual Mode of Action.

Angew Chem Int Ed Engl 2020 09 8;59(36):15532-15536. Epub 2020 Jul 8.

Institute of Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, 14195, Berlin, Germany.

In this study, we demonstrate the concept of "topology-matching design" for virus inhibitors. With the current knowledge of influenza A virus (IAV), we designed a nanoparticle-based inhibitor (nano-inhibitor) that has a matched nanotopology to IAV virions and shows heteromultivalent inhibitory effects on hemagglutinin and neuraminidase. The synthesized nano-inhibitor can neutralize the viral particle extracellularly and block its attachment and entry to the host cells. The virus replication was significantly reduced by 6 orders of magnitude in the presence of the reverse designed nano-inhibitors. Even when used 24 hours after the infection, more than 99.999 % inhibition is still achieved, which indicates such a nano-inhibitor might be a potent antiviral for the treatment of influenza infection.
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http://dx.doi.org/10.1002/anie.202004832DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7497169PMC
September 2020

Well-Defined Diblock Poly(ethylene glycol)--Poly(ε-caprolactone)-Based Polymer-Drug Conjugate Micelles for pH-Responsive Delivery of Doxorubicin.

Materials (Basel) 2020 Mar 26;13(7). Epub 2020 Mar 26.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.

Nanoparticles have emerged as versatile carriers for various therapeutics and can potentially treat a wide range of diseases in an accurate and disease-specific manner. Polymeric biomaterials have gained tremendous attention over the past decades, owing to their tunable structure and properties. Aliphatic polyesters have appealing attributes, including biodegradability, non-toxicity, and the ability to incorporate functional groups within the polymer backbone. Such distinctive properties have rendered them as a class of highly promising biomaterials for various biomedical applications. In this article, well-defined alkyne-functionalized poly(ethylene glycol)--poly(ε-caprolactone) (PEG--PCL) diblock copolymer was synthesized and studied for pH-responsive delivery of doxorubicin (DOX). The alkyne-functionalized PEG--PCL diblock copolymer was prepared by the synthesis of an alkyne-functionalized ε-caprolactone (CL), followed by ring-opening polymerization (ROP) using PEG as the macroinitiator. The alkyne functionalities of PEG--PCL were modified through copper(I)-catalyzed alkyne-azide cycloaddition (CuAAC) click reaction to graft aldehyde (ALD) groups and obtain PEG--PCL--ALD. Subsequently, DOX was conjugated on PEG--PCL--ALD through the Schiff base reaction. The resulting PEG--PCL--DOX polymer-drug conjugate (PDC) self-assembled into a nano-sized micellar structure with facilitated DOX release in acidic pH due to the pH-responsive linkage. The nanostructures of PDC micelles were characterized using transmission electron microscopy (TEM) and dynamic light scattering (DLS). In vitro studies of the PDC micelles, revealed their improved anticancer efficiency towards MCF-7 cells as compared to free DOX.
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http://dx.doi.org/10.3390/ma13071510DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7177263PMC
March 2020

Metal-Organic Framework/Ag-Based Hybrid Nanoagents for Rapid and Synergistic Bacterial Eradication.

ACS Appl Mater Interfaces 2020 Mar 12;12(12):13698-13708. Epub 2020 Mar 12.

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, China.

Recent emerged metal-organic frameworks (MOFs), as superior drug carriers, provide novel strategies to combat pathogenic bacterial infections. Although various antibacterial metal ions can be easily introduced in MOFs for chemical bacterial ablation, such a single-model bactericidal method suffers from high-dose use, limited antibacterial efficiency, and slow sterilization rate. Hence, developing a dual bactericidal system is urgently required. Herein, we report an MOF/Ag-derived nanocomposite with efficient metal-ion-releasing capability and robust photo-to-thermal conversion effect for synergistic sterilization. The MOF-derived nanocarbon consisting of metallic zinc and a graphitic-like carbon framework is first synthesized, and then Ag nanoparticles (AgNPs) are evenly introduced via the displacement reaction between Zn and Ag. Upon near-infrared irradiation, the fabricated nanoagents can generate massive heat to destroy bacterial membranes. Meanwhile, abundant Zn and Ag ions are released to make chemical damage to bacterial intracellular substances. Systematic antibacterial experiments reveal that such dual-antibacterial effort can endow the nanoagents with nearly 100% bactericidal ratio for highly concentrated bacteria at a very low dosage (0.16 mg/mL). Furthermore, the nanoagents exhibit less cytotoxicity, which provides potential possibilities for the applications in the biological field. assessment indicates that the nanocomposites can realize rapid and safe wound sterilization and are expected to be an alternative to antibiotics. Overall, we present an easily fabricated structure-engineered nanocomposite with chemical and photothermal effects for broad-spectrum bacterial sterilization.
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http://dx.doi.org/10.1021/acsami.0c01666DOI Listing
March 2020

PEGylated Amine-Functionalized Poly(ε-caprolactone) for the Delivery of Plasmid DNA.

Materials (Basel) 2020 Feb 18;13(4). Epub 2020 Feb 18.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY 14260, USA.

As a promising strategy for the treatment of various diseases, gene therapy has attracted increasing attention over the past decade. Among various gene delivery approaches, non-viral vectors made of synthetic biomaterials have shown significant potential. Due to their synthetic nature, non-viral vectors can have tunable structures and properties by using various building units. In particular, they can offer advantages over viral vectors with respect to biosafety and cytotoxicity. In this study, a well-defined poly(ethylene glycol)--poly(α-(propylthio-,-diethylethanamine hydrochloride)-ε-caprolactone) diblock polymer (PEG--CPCL) with one poly(ethylene glycol) (PEG) block and one tertiary amine-functionalized cationic poly(ε-caprolactone) (CPCL) block, as a novel non-viral vector in the delivery of plasmid DNA (pDNA), was synthesized and studied. Despite having a degradable polymeric structure, the polymer showed remarkable hydrolytic stability over multiple weeks. The optimal ratio of the polymer to pDNA for nanocomplex formation, pDNA release from the nanocomplex with the presence of heparin, and serum stability of the nanocomplex were probed through gel electrophoresis. Nanostructure of the nanocomplexes was characterized by DLS and TEM imaging. Relative to CPCL homopolymers, PEG--CPCL led to better solubility over a wide range of pH. Overall, this work demonstrates that PEG--CPCL possesses a range of valuable properties as a promising synthetic vector for pDNA delivery.
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http://dx.doi.org/10.3390/ma13040898DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7079624PMC
February 2020

Construction of Kevlar nanofiber/graphene oxide composite beads as safe, self-anticoagulant, and highly efficient hemoperfusion adsorbents.

J Mater Chem B 2020 03;8(9):1960-1970

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, China.

Recently emerged hemoperfusion absorbents, e.g. ion-exchange resin, activated carbon, and other porous materials, provide numerous novel possibilities to cure chronic liver failure (CLF) and renal failure (CRF). However, the limited adsorption performance and unsatisfactory blood compatibility significantly impede the development of the absorbents. Hence, designing safe and self-anticoagulant hemoperfusion absorbents with robust toxin clearance remains a considerable challenge. Here, brand new Kevlar-based composite gel beads for hemoperfusion are prepared by interface assembly based on π-π interaction. First, Kevlar nanofiber-graphene oxide (K-GO) beads are produced by liquid-liquid phase separation. Then, sodium p-styrenesulfonate (SS) is adsorbed onto the K-GO interface by π-π interaction and initiated to achieve the composite gel (K-GO/PSS) beads with an interfacial crosslinked structure. Such composite gel beads possess superior mechanical strength and self-anticoagulation capability, owing to the dual-network structure and heparin-mimicking gel structure, respectively. Furthermore, the K-GO/PSS beads show robust adsorption capacities for different kinds of toxins due to their strong charge and π-π interactions. A simulated hemoperfusion experiment in vitro demonstrates that the concentrations of the toxins in the blood can be restored to normal values within 30 minutes. In general, we envision that such composite gel beads will provide new strategies for future clinical CLF and CRF treatments.
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http://dx.doi.org/10.1039/c9tb02789kDOI Listing
March 2020

Super-tough poly (l-lactide) materials: Reactive blending with maleic anhydride grafted starch and poly (ethylene glycol) diacrylate.

Int J Biol Macromol 2019 Sep 20;136:1069-1075. Epub 2019 Jun 20.

Textile Institute, Sichuan University, Chengdu 610065, China. Electronic address:

Super-tough poly (l-lactide) (PLLA) without compromising its biodegradability and biocompatibility was fabricated by reactive blending with PLLA and maleic anhydride grafted starch (MS)/poly (ethylene glycol) diacrylate (PEGDA). PEGDA as reactive compatibilizer exhibits higher compatibilization efficiency and significant plasticization effect in PLLA matrix. Fourier transform infrared spectroscopy (FT-IR) confirmed that PEGDA monomer successfully located at the molecules of MS and some interesterification reactions occurred between PEGDA and PLLA. The ductility of PLLA materials were significantly improved, for example, the elongation of break increased to 298% at the optimum PLLA/MS/PEGDA content. Dynamic mechanical thermal analysis (DMTA) demonstrated the glass transition temperature of blends decreased with the contents of MS/PEGDA increasing. The differential scanning calorimeter (DSC) results revealed that cold crystallization temperature and melting temperature of blends were decreased with the augment of the contents of MS/PEGDA. Wide angle X-ray diffraction (WARD) and DSC certified that a high crystalline article was obtained through practical extrusion process, which could propagate shear yielding deformation to dissipate energy during tensile fracture. Scanning electron microscope (SEM) demonstrated that the blends with PEGDA did not exhibit a visible phase-separated morphology from cryogenic fractured surfaces compared with the blend without PEGDA.
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http://dx.doi.org/10.1016/j.ijbiomac.2019.06.141DOI Listing
September 2019

Linear-Dendritic Alternating Copolymers.

Angew Chem Int Ed Engl 2019 07 27;58(31):10572-10576. Epub 2019 Jun 27.

Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.

Herein, the design, synthesis, and characterization of an unprecedented copolymer consisting of alternating linear and dendritic segments is described. First, a 4th-generation Hawker-type dendron with two azide groups was synthesized, followed by a step-growth azide-alkyne "click" reaction between the 4th-generation diazido dendron and poly(ethylene glycol) diacetylene to create the target polymers. Unequal reactivity of the functional groups was observed in the step-growth polymerization. The resulting copolymers, with alternating hydrophilic linear and hydrophobic dendritic segments, can spontaneously associate into a unique type of microphase-segregated nanorods in water.
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http://dx.doi.org/10.1002/anie.201903402DOI Listing
July 2019

Metal-Organic-Framework-Derived 2D Carbon Nanosheets for Localized Multiple Bacterial Eradication and Augmented Anti-infective Therapy.

Nano Lett 2019 09 22;19(9):5885-5896. Epub 2019 May 22.

Department of Chemistry and Biochemistry , Freie Universität Berlin , Takustrasse 3 , 14195 Berlin , Germany.

Recently emerging graphene-based 2D nanoplatforms with multiple therapeutic modalities provide enormous opportunities to combat pathogenic bacterial infections. However, because these materials suffer from complicated synthesis, massive dosage requirements, and abundant nonlocalized heat, much more simplified, tunable, and localized eradication approaches are urgently required. Herein, we report on the fabrication of the metal-organic-framework (MOF)-derived 2D carbon nanosheets (2D-CNs) with phase-to-size transformation and localized bacterial eradication capabilities for augmented anti-infective therapy. The MOF-derived, ZnO-doped carbon on graphene (ZnO@G) is first synthesized and then anchored with phase transformable thermally responsive brushes (TRB) by in situ polymerization to yield the TRB-ZnO@G. The TRB-ZnO@G exhibits flexible 2D nanostructures, high photothermal activities, sustained Zn ions release, and ON-OFF switchable phase-to-size transformation abilities. Notably, the near-infrared-triggered formation of TRB-ZnO@G-bacteria aggregations enables localized massive Zn ions penetration, physical cutting, and hyperthermia killing, which synergistically enhance the disruption of bacterial membranes and intracellular substances. The obtained novel 2D-CNs not only present robust and localized multiple bacterial eradication capabilities with nearly 100% bactericidal efficiency at low concentrations but also possess rapid and safe skin wound disinfection via a short-time photothermal treatment without damaging normal skin tissues or causing accumulative toxicities, thus presenting great potential for broad-spectrum eradication of pathogenic bacteria.
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http://dx.doi.org/10.1021/acs.nanolett.9b01400DOI Listing
September 2019

Microwave pyrolysis valorization of used baby diaper.

Chemosphere 2019 Sep 10;230:294-302. Epub 2019 May 10.

School of Environmental Engineering, University of Seoul, Seoul, 02504, Republic of Korea. Electronic address:

Used baby diaper consists of a combination of decomposable cellulose, non-biodegradable plastic materials (e.g. polyolefins) and super-absorbent polymer materials, thus making it difficult to be sorted and separated for recycling. Microwave pyrolysis was examined for its potential as an approach to transform used baby diapers into value-added products. Influence of the key operating parameters comprising process temperature and microwave power were investigated. The pyrolysis showed a rapid heating process (up to 43 °C/min of heating rate) and quick reaction time (20-40 min) in valorizing the used diapers to generate pyrolysis products comprising up to 43 wt% production of liquid oil, 29 wt% gases and 28 wt% char product. Microwave power and operating temperature were observed to have impacts on the heating rate, process time, production and characteristics of the liquid oil and solid char. The liquid oil contained alkanes, alkenes and esters that can potentially be used as chemical additives, cosmetic products and fuel. The solid char contained high carbon, low nitrogen and free of sulphur, thus showing potential for use as adsorbents and soil additives. These observations demonstrate that microwave pyrolysis has great prospect in transforming used baby diaper into liquid oil and char products that can be utilised in several applications.
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http://dx.doi.org/10.1016/j.chemosphere.2019.05.054DOI Listing
September 2019

Downregulation of microRNA-92b-3p suppresses proliferation, migration, and invasion of gastric cancer SGC-7901 cells by targeting Homeobox D10.

J Cell Biochem 2019 10 20;120(10):17405-17412. Epub 2019 May 20.

Department of Surgical Oncology, Shannxi Provincial People's Hospital, Xi'an, Shaanxi, China.

To investigate the effect and mechanism of microRNA-92b-3p (miR-92b-3p) targeting Homeobox D10 (HOXD10) on proliferation, migration, and invasion of gastric cancer, we detected the expression of miR-92b-3p and HOXD10 in SGC-7901 cells. The effects of miR-92b-3p or HOXD10 on proliferation, migration, invasion, and matrix metalloproteinase (MMP)-2/9 expression in SGC-7901 cells were measured by the Cell Counting Kit-8 assay, Transwell assay, and Western blot, respectively. The results showed that miR-92b-3p expression was increased, and HOXD10 expression was decreased in SGC-7901 cells, compared with human normal gastric epithelial cells GES-1. Functional experiments demonstrated that cell proliferation, migration, invasion, and expression of MMP-2/9 in SGC-7901 cells were significantly inhibited by miR-92b-3p silencing and HOXD10 overexpression. Moreover, HOXD10 was a potential target gene of miR-92b-3p as evidenced by the TargetScan software and double luciferase reporter assay. In the rescue experiment, knockdown of HOXD10, accompanied by higher expression of MMP-2/9, could significantly eliminate the inhibitory effects of miR-92b-3p silencing on cell proliferation, migration, and invasion. In conclusion, miR-92b-3p is highly expressed in gastric cancer SGC-7901 cells, and interfering with its expression might inhibit SGC-7901 cell proliferation, migration, and invasion via downregulating MMP-2/9 expression and targeting HOXD10.
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http://dx.doi.org/10.1002/jcb.29005DOI Listing
October 2019

Doxorubicin-loaded FeO-ZIF-8 nano-composites for hepatocellular carcinoma therapy.

J Biomater Appl 2019 05 16;33(10):1373-1381. Epub 2019 Mar 16.

1 Department of Hepatobiliary Surgery, Institute of Advanced Surgical Technology and Engineering, Regenerative Medicine and Surgery Engineering Research Center of Shaanxi Province, The First Affiliated Hospital of Xi'an Jiaotong University, Xi'an, China.

Hepatocellular carcinoma (HCC) is one of the most common and malignant cancers and has no effective therapeutic approaches. Chemotherapeutic drug doxorubicin (DOX) is widely used for HCC therapy, but its application is limited by the clinical toxicity. In the present study, an FeO-ZIF-8 magnetic nano-composite was fabricated and used for DOX delivery for HCC therapy. The morphology, structure and property of FeO-ZIF-8 nano-composites were evaluated by scanning electron microscopy, transmission electron microscopy and N adsorption-desorption isotherms studies. The drug release from DOX@FeO-ZIF-8 was measured in pH 7.4 phosphate-buffered saline. The cellular uptake ability of DOX@FeO-ZIF-8 into hepatocarcinoma cell line (MHCC97H) was visualized with a confocal laser scanning microscope. The effects of FeO-ZIF-8, DOX and DOX@FeO-ZIF-8 against MHCC97H cells were evaluated by CCK-8 assay and flow cytometry assay. FeO-ZIF-8 nano-composites were synthesized and used as a nano-carrier for the delivery of DOX. Because of high drug loading property of ZIF-8, 1 mg FeO-ZIF-8 nano-composites loaded 120 μg DOX when DOX@FeO-ZIF-8 was synthesized in 30 mg/mL DOX solution. The cumulative DOX release curve showed a slow and sustained release pattern over time. The results of CCK-8 assay showed that FeO-ZIF-8 was nontoxic to MHCC97H cells, and DOX@FeO-ZIF-8 presented effective inhibiting effect on cell viability of MHCC97H cells. Cellular uptake assay showed that DOX@FeO-ZIF-8 accumulated in both cytoplasm and nuclei. Moreover, because of valid drug accumulation, DOX@FeO-ZIF-8 exhibited a good inducing effect on cell apoptosis of MHCC97H cells. In conclusion, based on the nontoxic and high drug loading capability of FeO-ZIF-8, DOX@FeO-ZIF-8 presented enhanced effects on HCC cells compared to free DOX, indicating its potential for the chemotherapy of HCC.
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http://dx.doi.org/10.1177/0885328219836540DOI Listing
May 2019