Poly(ethylene glycol)-poly(sulfamethazine-ester-urethane) based pH-/temperature-sensitive, biodegradable and injectable hydrogel for cationic protein delivery

Le Thai Minh Duy,V.H Giang Phan,Doo Sung Lee 한국고분자학회 2016 한국고분자학회 학술대회 연구논문 초록집 Vol.41 No.2

Bioinspired pH- and Temperature-Responsive Injectable Adhesive Hydrogels with Polyplexes Promotes Skin Wound Healing

Le, Thai Minh Duy,Duong, Huu Thuy Trang,Thambi, Thavasyappan,Giang Phan, V.H.,Jeong, Ji Hoon,Lee, Doo Sung American Chemical Society 2018 Biomacromolecules Vol.19 No.8

<P>Despite great potential, the delivery of genetic materials into cells or tissues of interest remains challenging owing to their susceptibility to nuclease degradation, lack of permeability to the cell membrane, and short in vivo half-life, which severely restrict their widespread use in therapeutics. To surmount these shortcomings, we developed a bioinspired in situ-forming pH- and temperature-sensitive injectable hydrogel depot that could control the delivery of DNA-bearing polyplexes for versatile biomedical applications. A series of multiblock copolymer, comprised of water-soluble poly(ethylene glycol) (PEG) and pH- and temperature-responsive poly(sulfamethazine ester urethane) (PSMEU), has been synthesized as in situ-forming injectable hydrogelators. The free-flowing PEG-PSMEU copolymer sols at high pH and room temperature (pH 8.5, 23 °C) were transformed to stable gel at the body condition (pH 7.4, 37 °C). Physical and mechanical properties of hydrogels, including their degradation rate and viscosity, are elegantly controlled by varying the composition of urethane ester units. Subcutaneous administration of free-flowing PEG-PSMEU copolymer sols to the dorsal region of Sprague-Dawley rats instantly formed hydrogel depot. The degradation of the hydrogel depot was slow at the beginning and found to be bioresorbable after two months. Cationic protein or DNA-bearing polyplex-loaded PEG-PSMEU copolymer sols formed stable gel and controlled its release over 10 days in vivo. Owing to the presence of urethane linkages, the PEG-PSMEU possesses excellent adhesion strength to wide range of surfaces including glass, plastic, and fresh organs. More importantly, the hydrogels effectively adhered on human skin and peeled easily without eliciting an inflammatory response. Subcutaneous implantation of PEG-PSMEU copolymer sols effectively sealed the ruptured skin, which accelerated the wound healing process as observed by the skin appendage morphogenesis. The bioinspired in situ-forming pH- and temperature-sensitive injectable adhesive hydrogel may provide a promising platform for myriad biomedical applications as controlled delivery vehicle, adhesive, and tissue regeneration.</P> [FIG OMISSION]</BR>

Bioinspired pH- and Temperature-Responsive Injectable Adhesive Hydrogels with Polyplexes Promotes Skin Wound Healing

Thai Minh Duy Le,Huu Thuy Trang Duong,Thavasyappan Thambi,V. H. Giang Phan,정지훈,이두성 한국고분자학회 2019 한국고분자학회 학술대회 연구논문 초록집 Vol.44 No.2

A Novel Injectable pH–Temperature Sensitive Hydrogel Containing Chitosan–Insulin Electrosprayed Nanosphere Composite for an Insulin Delivery System in Type I Diabetes Treatment

Thuy An Trinh,Thai Minh Duy Le,Hoang Gia Vinh Ho,Thi Cam Thach To,Vu Viet Linh Nguyen,Dai Phu Huynh,Doo Sung Lee 한국고분자학회 2021 한국고분자학회 학술대회 연구논문 초록집 Vol.46 No.1

Faculty of Materials Technology, Ho Chi Minh University of Technology (HCMUT)/Vietnam National University Ho Chi Minh City; ¹School of Chemical Engineering and Theragnostic Macromolecules Research Center, Sungkyunkwan University; ²Vietnam National University Ho Chi Minh City/National Key Laboratory of Polymer and Composite Materials, Ho Chi Minh University of Technology, Vietnam National University; ³Faculty of Materials Technology, Ho Chi Minh University of Technology (HCMUT)/ Vietnam National University Ho Chi Minh City/Research Center for Polymeric Materials, Ho Chi Minh University of Technology, Vietnam National University In this research, a novel insulin composite delivery system was prepared and characterized. Insulin drug was loading in chitoshan nanospheres using electrospraying method, a pH- and temperature-sensitive biodegradable hydrogel, which is an oligomer serine-poly(lactide)-poly(ethylene glycol)-poly (lactide)-oligomer serine (OS-PLA-PEG-PLA-OS) pentablock copolymer was used as a matrix to containing chitosan–insulin electro sprayed nanospheres (CIN). The properties of the OS-PLA-PEG-PLA-OS pentablock copolymer and the chitosan–insulin nanoparticles such as sol-gel transition, degradation in vitro and in vivo were characterized. The results showed that the chitosan–insulin nanospheres uniformly distributed in the matrix had a reinforcing effect on the mechanical properties and prolonged the degradation time of the hydrogel depot under body conditions. In addition, the cytotoxicity experiment results indicate that the composite could be used as a biomaterial for drug delivery system. The composite solutions accommodating different concentrations of the chitosan–insulin nanospheres were subcutaneously injected into induced diabetic BALB/c mice to study the in vivo insulin-release profile. The result showed that insulin concentrations in blood plasma were maintained at a steady-state level. Furthermore, the bio-properties of the insulin were retained and it showed a blood glucose level reducing effect for more than 60 hours after injection to a streptozotocin (STZ)-induced diabetic mouse model. The results suggested that this injectable pH–temperature sensitive hydrogel containing chitosan– insulin electro sprayed nanosphere composites has promising potential applications for type 1 diabetes treatment.

High-Performance Schottky Diode Gas Sensor Based on the Heterojunction of Three-Dimensional Nanohybrids of Reduced Graphene Oxide–Vertical ZnO Nanorods on an AlGaN/GaN Layer

Minh Triet, Nguyen,Thai Duy, Le,Hwang, Byeong-Ung,Hanif, Adeela,Siddiqui, Saqib,Park, Kyung-Ho,Cho, Chu-Young,Lee, Nae-Eung American Chemical Society 2017 ACS APPLIED MATERIALS & INTERFACES Vol.9 No.36

<P>A Schottky diode based on a heterojunction of three-dimensional (3D) nanohybrid materials, formed by hybridizing reduced graphene oxide (RGO) with epitaxial vertical zinc oxide nanorods (ZnO NRs) and Al0.27GaN0.73(similar to 25 nm)/GaN is presented as a new class of high-performance chemical sensors. The RGO nanosheet layer coated on the ZnO NRs enables the formation of a direct Schottky contact with the AlGaN layer. The sensing results of the Schottky diode with respect to NO2, SO2, and HCHO gases exhibit high sensitivity (0.88-1.88 ppm(-1)), fast response (similar to 2 min), and good reproducibility down concentration levels at room temperature. The sensing mechanism of the Schottky diode can be explained by modulation of the reverse saturation current due to the change in thermionic emission carrier transport caused by ultrasensitive changes in the Schottky barrier of a van der Waals heterostructure between RGO and AlGaN layers upon interaction with gas molecules. Advances in the design of a Schottky diode gas sensor based on the heterojunction of high-mobility two-dimensional electron gas channel and highly responsive 3D-engineered sensing nanomaterials have potential not only for the enhancement of sensitivity and selectivity but also for improving operation capability at room temperature.</P>

Synthesis of a Novel Fluorescent Cyanide Chemosensor Based on Photoswitching Poly(pyrene-1-ylmethyl-methacrylate-randommethyl methacrylate-random-methacrylate spirooxazine)

Hoan Minh Tran,Tam Huu Nguyen,Viet Quoc Nguyen,Phuc Huynh Tran,Linh Duy Thai,Thuy Thu Truong,Le-Thu T. Nguyen,Ha Tran Nguyen 한국고분자학회 2019 Macromolecular Research Vol.27 No.1

The photoswitching poly(pyrene-1-ylmethyl-methacrylate-random-methyl methacrylate-random-methacrylate spirooxazine) was synthesized via atom transfer radical polymerization and characterized by proton nuclear magnetic resonance (1H NMR), gel permeation chromatography (GPC), Fourier transform infrared (FTIR) spectroscopy, UV-visible spectroscopy, and differential scanning calorimetry (DSC). The obtained copolymer exhibited the capability of erasable and rewritable photoimaging, making it a potential candidate for optical data storage materials. Moreover, the copolymer also showed the sensing ability for cyanide anions effect in aqueous solutions.

Tumor acidity and CD44 dual targeting hyaluronic acid-coated gold nanorods for combined chemo- and photothermal cancer therapy

Li, Yi,Duy Le, Thai Minh,Nam Bui, Quang,Yang, Hong Yu,Lee, Doo Sung Elsevier 2019 Carbohydrate polymers Vol.226 No.-

<P><B>Abstract</B></P> <P>In this work, tumor acidity and CD44 dual targeting hyaluronic acid-coated gold nanorods (AuNRs) are investigated for combined chemo- and photothermal cancer therapy. Low molecular weight hyaluronic acid (LMWHA) is conjugated with pH-sensitive groups for pH-induced aggregation and lipoic acid for coating of AuNRs. By changing pH-sensitive groups with different pKa values, pH-sensitivity of modified LMWHA can be tuned. After coating modified LMWHA onto AuNRs, biocompatibility of the AuNRs is significantly improved. These LMWHA-coated AuNRs can gradually aggregate under slightly acidic conditions, making them favorable for accumulation at acidic tumor sites. Surface LMWHA allows the nanocomposites to be selectively uptaken by CD44-expressing cancer cells, and AuNRs endows the nanocomposites with excellent photothermal ability. Loading of doxorubicin, a chemical drug, provides the LMWHA-coated AuNRs synergistic cancer cell-killing (<I>in vitro</I>) and tumor growth inhibiting (<I>in vivo</I>) ability. Taken together, these results demonstrate that this multifunctional nanosystem with pH-induced aggregation and CD44 targeting has potential for combined chemo- and photothermal cancer therapy.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Conjugation of pH-sensitive groups induces acidity-triggered aggregation. </LI> <LI> Surface coating of hyaluronic acid allows selective tumor targeting of nanoparticles. </LI> <LI> Co-delivery of chemical drugs and gold nanorods enables combined cancer therapy. </LI> </UL> </P>

Development of bioresorbable smart injectable hydrogels based on thermo-responsive copolymer integrated bovine serum albumin bioconjugates for accelerated healing of excisional wounds

V. H. Giang Phan,Thai Minh Duy Le,고피나단 자나르다난,Phuong-Khanh Thi Ngo,이두성,Thavasyappan Thambi 한국공업화학회 2021 Journal of Industrial and Engineering Chemistry Vol.96 No.-

One of the major challenges in wound healing is the development of suitable hydrogels that areinjectable, biocompatible with multiple functionalities and properties such as high mechanical, tissueadhesiveness, and swelling properties. However, these hydrogels should not elicit any immunologicalresponse and synthesis steps should be easier and tunable according to the requirements. Consideringthese properties, we synthesized a thermo-sensitive triblock copolymer consisting of bovine serumalbumin (BSA) protein capable of leveraging the needs for a proper wound closure and tissueregeneration on excisional injuries. Firstly, the triblock copolymer consisting of poly(e-caprolactone-colactide)-b-poly(ethylene glycol)-b-poly(e-caprolactone-co-lactide (PCLA) was synthesized and then thecopolymer was grafted with BSA to yield BSA-PCLA bioconjugates. Aqueous solutions of free-flowingbioconjugate sol at room temperature can transform to gel at physiological temperature with highviscoelastic properties. Subcutaneous injection of BSA-PCLA bioconjugate sol into the back of Sprague-Dawley rats formed gel immediately and found to be bioresorbable after 5 weeks without significanttoxicity at implantation sites. BSA-PCLA bioconjugate gel exhibited good adhesive property to majororgans including liver, heart, and spleen when compared with control PCLA gel. When tested for in vivowound closure trials, the BSA-PCLA gels showed rapid wound contraction compared to the PCLA and thecontrol. The increased angiogenesis and collagen deposition were confirmed from the histological studiesof the samples. These highly adhesive, biocompatible, biodegradable, thermos-sensitive bioconjugategels show promising potential in wound healing and tissue regeneration without any additionalbiofactors or inorganic nanoparticles.

Triple-, Double-, and Single-Shelled Hollow Spheres of Sulfonated Microporous Organic Network as Drug Delivery Materials

Jang, June Young,Le, Thai Minh Duy,Ko, Ju Hong,Ko, Yoon-Joo,Lee, Sang Moon,Kim, Hae Jin,Jeong, Ji Hoon,Thambi, Thavasyappan,Lee, Doo Sung,Son, Seung Uk American Chemical Society 2019 Chemistry of materials Vol.31 No.2

[FIG OMISSION]</BR>

A durable and stable piezoelectric nanogenerator with nanocomposite nanofibers embedded in an elastomer under high loading for a self-powered sensor system

Siddiqui, Saqib,Kim, Do-Il,Roh, Eun,Duy, Le Thai,Trung, Tran Quang,Nguyen, Minh Triet,Lee, Nae-Eung Elsevier 2016 Nano energy Vol.30 No.-

<P><B>Abstract</B></P> <P>Practical usage of piezoelectric nanogenerators (PENGs) under heavy loading environments for high power generation, such as smart shoes, has been limited due to the low mechanical endurance of many piezoelectric materials. Durability and performance under harsh environments are a stumbling block for the practical application of PENGs. Synthesis of piezoelectrically enhanced nanofibers electrospun from nanocomposite of barium titanate nanoparticles (BT NPs) dispersed in poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) enables successful fabrication of a robust, efficient, flexible and lead-free PENG. A nanofiber PENG (nf-PENG) fabricated by embedding nanocomposite nanofibers in an elastomer film is demonstrated for biomechanical energy harvesting and storage during walking. When placed inside of a shoe, a nf-PENG loaded with 15wt% BT NPs can generate an output of 25V at a walking frequency of 0.6Hz with high mechanical durability under very high loads (600N). This can charge a 4.7µF capacitor after approximately 72 steps. The stored charge can operate a strain sensor without any external power supply. The high performance of the nf-PENG is mainly attributed to the self-poled nanocomposite nanofibers. Additionally, embedding the nanofibers into an elastomer provided high durability by protecting the nanofibers from mechanical damage. Furthermore, the devices small form factor, flexibility, and transparency make this nf-PENG suitable for applications in wearable electronics, where aesthetics and comfort are also desired (in addition to performance). This work demonstrates the possibility of highly durable, efficient, and self-powered wearable sensing systems that can work under extreme environments.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Lead-free piezoelectric nanocomposite nanofibers. </LI> <LI> High durability under harsh environments and high loadings. </LI> <LI> Harvesting and storing biomechanical energy during walking. </LI> <LI> Self-powered system. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>A highly durable, efficient and flexible piezoelectric nanogenerator, comprised of piezoelectric nanocomposite nanofibers embedded into an elastomer, was designed for energy harvesting under heavy loading conditions. The high resistance of the generator to ambient conditions for prolonged periods of time, as well as resistance to damage under heavy loading conditions, enabled the efficient harvest of bio-mechanical energy during human walking. This energy could be stored in a capacitor to create a self-powered sensor system. This approach may help enable practical applications of piezoelectric nanogenerators in wearable systems.</P> <P>[DISPLAY OMISSION]</P>