Publications by authors named "Meifang Zhu"

149 Publications

Transforming a Sword into a Knife: Persistent Phototoxicity Inhibition and Alternative Therapeutical Activation of Highly-Photosensitive Phytochlorin.

ACS Nano 2021 Dec 1. Epub 2021 Dec 1.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

The phototoxicity of photosensitizers (PSs) is a double-edged sword with one edge beneficial for destroying tumors while the other is detrimental to normal tissues, and the conventional "OFF-ON" strategy provides temporary inhibition so that phototoxicity would come sooner or later due to the inevitable retention and transformation of PSs . We herein put forward a strategy to convert "double-edged sword" PSs into "single-edged knife" ones with simultaneously persistent phototoxicity inhibition and alternative multiple therapeutical activation. The Chlorin e6 (Ce6) as the PS model directly assembles with Cu ions into nanoscale frameworks (nFs) whose Cu-coordination includes both carboxyl groups and a porphyrin ring of Ce6 instead of Fe/Mn-coordination with only carboxyl groups. Compared to the high phototoxicity of Ce6, the nFs exhibit efficient energy transfer due to the dual-coordination of paramagnetic Cu ions and the aggregation, achieving the persistent and high phototoxicity inhibition rate of >92%. Alternatively, the nFs not only activate a high photoacoustic contrast and near-infrared (NIR)-driven photothermal efficacy (3.5-fold that of free Ce6) due to the aggregation-enhanced nonradiative transition but also initiate tumor microenvironment modulation, structure disassembly, and chemodynamic effect by Cu ions. Given these merits, the nFs achieve long-term biosecurity, no retina injury under sunlight, and a higher therapeutical output than the photodynamic effect of Ce6. This work presents a possibility of converting numerous highly phototoxic porphyrins into safe and efficient ones.
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http://dx.doi.org/10.1021/acsnano.1c07241DOI Listing
December 2021

Biomass-Derived, Highly Conductive Aqueous Inks for Superior Electromagnetic Interference Shielding, Joule Heating, and Strain Sensing.

ACS Appl Mater Interfaces 2021 Nov 19. Epub 2021 Nov 19.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Conductive composite inks are widely used in various applications such as flexible electronics. However, grand challenges still remain associated with their relatively low electrical conductivity and require heavy use of organic solvents, which may limit their high performance in broad applications and cause environmental concerns. Here, we report a generalized and eco-friendly strategy to fabricate highly conductive aqueous inks using silver nanowires (AgNWs) and biomass-derived organic salts, including succinic acid-chitosan (SA-chitosan) and sebacic acid-chitosan. SA-chitosan/AgNW composite coatings can be prepared by directly casting conductive aqueous inks on various substrates, followed by subsequently heating for cross-linking. The composite coatings exhibit an ultrahigh electrical conductivity up to 1.4 × 10 S/cm, which are stable after being treated with various organic solvents and/or kept at a high temperature of 150 °C, indicating their high chemical and thermal resistance. The flexibility and performance durability of these composite coatings were demonstrated by a suite of characterization methods, including bending, folding, and adhesion tests. Moreover, a high electromagnetic interference shielding (EMI) effectiveness of 73.3 dB is achieved for SA-chitosan/AgNW composite coatings at a thickness of only 10 μm due to the ultrahigh electrical conductivity. Additionally, we further demonstrated that such conductive composite inks can be used for fabricating functional textiles for a variety of applications with high performance, such as EMI shielding, Joule heating, and strain sensing. The robust and highly conductive inks prepared by this simple and environmental-friendly method hold great promise as important material candidates for the potential large-scale manufacturing of flexible and wearable electronics.
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http://dx.doi.org/10.1021/acsami.1c17170DOI Listing
November 2021

Organic/Inorganic Hybrid Fibers: Controllable Architectures for Electrochemical Energy Applications.

Adv Sci (Weinh) 2021 Nov 11;8(22):e2102859. Epub 2021 Oct 11.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, P. R. China.

Organic/inorganic hybrid fibers (OIHFs) are intriguing materials, possessing an intrinsic high specific surface area and flexibility coupled to unique anisotropic properties, diverse chemical compositions, and controllable hybrid architectures. During the last decade, advanced OIHFs with exceptional properties for electrochemical energy applications, including possessing interconnected networks, abundant active sites, and short ion diffusion length have emerged. Here, a comprehensive overview of the controllable architectures and electrochemical energy applications of OIHFs is presented. After a brief introduction, the controllable construction of OIHFs is described in detail through precise tailoring of the overall, interior, and interface structures. Additionally, several important electrochemical energy applications including rechargeable batteries (lithium-ion batteries, sodium-ion batteries, and lithium-sulfur batteries), supercapacitors (sandwich-shaped supercapacitors and fiber-shaped supercapacitors), and electrocatalysts (oxygen reduction reaction, oxygen evolution reaction, and hydrogen evolution reaction) are presented. The current state of the field and challenges are discussed, and a vision of the future directions to exploit OIHFs for electrochemical energy devices is provided.
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http://dx.doi.org/10.1002/advs.202102859DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8596128PMC
November 2021

Enhancing the Electrochemical Performance of Sodium-Ion Batteries by Building Optimized NiS /NiSe Heterostructures.

Small 2021 Nov 7;17(45):e2104186. Epub 2021 Oct 7.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, P. R. China.

NiS Se nanosheets closely attached to the internal surface of hollow mesoporous carbon sphere (HMCS) to form a NiS Se nanosheets embedded in HMCS ([email protected]) composite as the anode of sodium ion batteries (SIBs) is reported by a facile synthesis route. The anode exhibits a superior reversible capacity (520 mAh g at 0.1 A g ) impressive coulombic efficiency (CE) of up to 95.3%, a high rate capacity (353 mAh g at 5.0 A g ), excellent capacity retention at high current density (95.6%), and high initial coulombic efficiency (ICE) (95.1%). Firstly, the highest ICE for NiS /NiSe -based anode can be ascribed to ultrathin layered structure of NiS Se nanosheet and highly efficient electron transfer between the active material and HMCS. Secondly, the optimized NiS /NiSe heterostructure at the nanoscale of the inside HMCS is formed after the first discharge/charge cycles, which can provide rich heterojunction interfaces/boundaries of sulfide/selenides to offer faster Na pathways, decrease the Na diffusion barriers, increase electronic conductivity, and limit the dissolution of polysulfides or polyselenides in the electrolyte. Finally, the hollow structure of the HMCS accommodates the volume expansion, prevents the pulverization and aggregation issues of composite materials, which can also promote outstanding electrochemical performance.
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http://dx.doi.org/10.1002/smll.202104186DOI Listing
November 2021

A baicalin-loaded coaxial nanofiber scaffold regulated inflammation and osteoclast differentiation for vascularized bone regeneration.

Bioact Mater 2022 Feb 30;8:559-572. Epub 2021 Jun 30.

Research Center for Nano-Biomaterials, Analytical and Testing Center, Sichuan University, Chengdu, 610064, PR China.

We demonstrate a simple, effective and feasible method to address the shrinkage of Poly (lactic--glycolic acid) (PLGA) through a core-shell structure fiber strategy. The results revealed that introducing size-stable poly-caprolactone (PCL) as the core fiber significantly improved the PLGA-based fibrous scaffold's dimensional maintenance. We further utilized fish collagen to modify the PLGA shell layer (PFC) of coaxial fibers and loaded baicalin (BA) into the PCL core layer (PCL-BA) to endow fibrous scaffold with more functional biological cues. The PFC/PCL-BA fibrous scaffold promoted the osteogenic differentiation of bone mesenchymal stem cells and stimulated the RAW264.7 cells to polarize into a pro-reparative phenotype. Importantly, the study demonstrated that the PFC/PCL-BA scaffold could regulate inflammation and osteoclast differentiation, favor neovascularization and bone formation. This work tactfully combined PLGA and PCL to establish a drug release platform based on the core-shell fibrous scaffold for vascularized bone regeneration.
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http://dx.doi.org/10.1016/j.bioactmat.2021.06.028DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8436066PMC
February 2022

Hierarchical Photothermal Fabrics with Low Evaporation Enthalpy as Heliotropic Evaporators for Efficient, Continuous, Salt-Free Desalination.

ACS Nano 2021 Jul 26. Epub 2021 Jul 26.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Shanghai Belt and Road Joint Laboratory of Advanced Fiber and Low-Dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Solar-driven seawater evaporation is usually achieved on floating evaporators, but the performances are substantially limited by high evaporation enthalpy, solid salt crystallization, and reduced evaporation due to inclined sunlight. To solve these problems, we fabricated hierarchical [email protected] sulfide ([email protected]) fabrics and proposed a prototype of heliotropic evaporator. Hierarchical [email protected] fabrics show significantly decreased water-evaporation enthalpy (1956.32 kJ kg, 40 °C), compared with that of pure water (2406.17 kJ kg, 40 °C), because of the disorganization of the hydrogen bonds at the CuS interfaces. Based on this fabric, a heliotropic evaporation model was developed, where seawater slowly flows from high to low in the fabric. Under solar irradiation (1.0 kW m), this model exhibits a high-rate evaporation (∼2.27 kg m h) and saturated brine production without solid salt crystallization. In particular, under inclined sunlight (angle range: from -90° to +90°), the heliotropic model retains an almost unchanged solar evaporation rate, whereas the floating model shows severe evaporation reduction (83.9%). Therefore, our study provides a strategy for reducing the evaporation enthalpy, maximally utilizing solar energy and continuous salt-free desalination.
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http://dx.doi.org/10.1021/acsnano.1c01900DOI Listing
July 2021

Ultralow Resistance Two-Stage Electrostatically Assisted Air Filtration by Polydopamine Coated PET Coarse Filter.

Small 2021 08 26;17(33):e2102051. Epub 2021 Jul 26.

Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.

Airborne particulate matters (PM) pose serious health threats to the population, and efficient filtration is needed for indoor and vehicular environments. However, there is an intrinsic conflict between filtration efficiency, air resistance, and service life. In this study, a two-stage electrostatically assisted air (EAA) filtration device is designed and the efficiency-air resistance-filter life envelope is significantly improved by a thin coating of polydopamine (PDA) on the polyethylene terephthalate (PET) coarse filter by in situ dopamine polymerization. The 8 mm thick EAA [email protected] filter has a high filtration efficiency of 99.48% for 0.3 µm particles, low air resistance of 9.5 Pa at a filtration velocity of 0.4 m s , and steady performance up to 30 d. Compared with the bare PET filter, the penetration rate for 0.3 µm particles is lowered by 20×. The coated PDA is of submicron thickness, 10  × the gap distance between filter fibers, so low air resistance could be maintained. The filter shows steadily high filtration efficiency and an acceptable increase of air resistance and holds nearly as many particles as its own weight in a 30 day long-term test. The working mechanism of the EAA coarse filter is investigated, and the materials design criteria are proposed.
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http://dx.doi.org/10.1002/smll.202102051DOI Listing
August 2021

Evaluation of a novel tilapia-skin acellular dermis matrix rationally processed for enhanced wound healing.

Mater Sci Eng C Mater Biol Appl 2021 Aug 21;127:112202. Epub 2021 May 21.

Shanghai Engineering Research Center of Nano-Biomaterials and Regenerative Medicine, College of Chemistry, Chemical Engineering and Biotechnology, Donghua University, Shanghai 201620, PR China. Electronic address:

Acellular Dermal Matrix (ADM) is mainly made with human or porcine skins and has the risk of zoonotic virus transmission. The fish skin-derived ADM could overcome the shortcoming. Fish skin acellular matrix has been used as wound dressing, but there is few systematic studies on tilapia-skin acellular dermal matrix (TS-ADM). In the present study, a novel TS-ADM was made by an alkaline decellularization process and γ-irradiation. The physical properties, biocompatibility, pre-clinical safety and wound healing activity of TS-ADM were systematically evaluated for its value as a functionally bioactive wound dressing. Histopathological analysis (hematoxylin and eosin staining, 4,6-diamidino-2-phenylindole (DAPI) staining) and DNA quantification both proved that the nuclear components of tilapia skin were removed sufficiently in TS-ADM. Compared to the commercial porcine acellular dermal matrix (DC-ADM), TS-ADM has distinctive features in morphology, thermal stability, degradability and water vapor transmission. TS-ADM was more readily degradable than DC-ADM in vitro and in vivo. In both rat and mini-pig skin wound healing experiments, TS-ADM was shown to significantly promote granulation growth, collagen deposition, angiogenesis and re-epithelialization, which may be attributed to the high expression of transforming growth factor-beta 1 (TGF-β1), alpha-smooth muscle actin (α-SMA) and CD31. Herein, the novel TS-ADM, used as a low-cost bioactive dressing, could form a microenvironment conducive to wound healing.
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http://dx.doi.org/10.1016/j.msec.2021.112202DOI Listing
August 2021

Activated Carbon Nanotube Fiber Fabric as a High-Performance Flexible Electrode for Solid-State Supercapacitors.

ACS Appl Mater Interfaces 2021 Jun 11;13(24):28433-28441. Epub 2021 Jun 11.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, 2999 North Renmin Road, Shanghai 201620, China.

Owing to their features of excellent mechanical flexibility, high conductivity, and light weight, carbon-based fiber fabrics (CBFFs) are highly attractive as flexible electrodes for flexible solid-state supercapacitors (SCs). However, the achieved areal capacitance of most CBFFs is still unsatisfactory. Carbon nanotube fiber fabric (CNTFF) is a new kind of CBFF and could provide a potential alternative to high-performance flexible electrodes. Herein, we report the activation of CNTFF using a facile thermal oxidation and acid treatment process. The activated CNTFF shows an exceptional combination of large areal capacitance (1988 mF cm at 2 mA cm), excellent rate performance (45% capacitance reservation at 100 mA cm), and outstanding cycle life (only 3% capacitance decay after 10,000 cycles). The constructed solid-state SC reaches a maximum energy density of 143 μWh cm at 1000 μW cm and a maximum power density of 30,600 μW cm at 82 μWh cm. Additionally, this device possesses good rate performance along with superb cycle stability and excellent mechanical flexibility under various bending conditions. Our present work therefore offers a new opportunity in developing high-performance flexible electrodes for flexible energy storage.
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http://dx.doi.org/10.1021/acsami.1c02758DOI Listing
June 2021

Synthesis and Characterization of Methacrylate-Functionalized Betulin Derivatives as Antibacterial Comonomer for Dental Restorative Resins.

ACS Biomater Sci Eng 2021 07 11;7(7):3132-3140. Epub 2021 Jun 11.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Secondary caries is the primary cause of composite restoration failures, resulting from marginal leakage and bacterial accumulation in the oral environment. Antibacterial dental composites, especially antibacterial monomers, have emerged as a promising strategy to inhibit secondary caries, which is pivotal to prolonging the lifespan of dental restorations. In this work, monomethacrylate- and dimethacrylate-functionalized betulin derivatives (MBet and MBet) were synthesized via an esterification reaction and served as antibacterial comonomers to develop novel dental resin formulations, in which MBet and MBet were incorporated to partially or completely replace bisphenol A glycerolate dimethacrylate (Bis-GMA). The control resin was a mixture based on Bis-GMA and tri(ethyleneglycol) dimethacrylate (TEGDMA) with a weight ratio of 50:50 (5B5T). The effect of the resin compositions and the chemical structures of MBet and MBet on the rheology behavior, optical property, polymerization kinetics, mechanical performance, cell viability, and antibacterial activity of dental resins were systematically investigated. Among all materials, the 1MBet4B5T resin with 10 wt % substitution of Bis-GMA by MBet exhibited comparable viscosity, higher light transmittance, improved degree of conversion, and mechanical properties compared with 5B5T. After incubation for 24 h, this optimal resin also possessed the best antibacterial activity against , which had a significantly lower bacterial concentration (1.53 × 10 CFU/mL) than 5B5T (9.03 × 10 CFU/mL). Introducing betulin-based comonomers into dental resins is a potential strategy to develop antibacterial dental materials without sacrificing physical-mechanical properties.
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http://dx.doi.org/10.1021/acsbiomaterials.1c00563DOI Listing
July 2021

Core-shell structured [email protected]@SiO filler for radiopacity and ultra-low shrinkage dental composite resins.

J Mech Behav Biomed Mater 2021 09 28;121:104593. Epub 2021 May 28.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, PR China.

To overcome the interfacial problem between X-ray radiopaque ZrO fillers and polymer resin in dental composites, monodispersed [email protected]@SiO (SZS) microspheres with narrow size distribution were prepared by a controlled sol-gel method. In the presence of SiO coating layer over [email protected] (SZ) microspheres, they were easily silanized same as SiO microspheres. Ethoxylated bisphenol A dimethacrylate (EBPADMA) with a higher molecular weight and a lower viscosity was used as base resin monomer mixed with a low amount of diluent triethylene glycol dimethacrylate (TEGDMA). Additionally, the addition of a small amount of pore agent acetone dicarboxylic acid (ADCA) produced some voids, thereby effectively reducing the polymerization shrinkage of the resin. The prepared dental composites combining 52 wt% monodispersed silica microsphere, 20 wt% SZS microspheres, exhibited significantly enhanced capacity in radiopacity (higher than tooth enamel) and very low shrinkage (<0.1%). It also has better mechanical properties than resin composites filled with SiO microspheres, and its strength can meet practical applications. The properties of the radiopaque dental composite were to be further tuned by varying the amount of SZS microspheres contents, and the radiopaque resin has an advantage over the commercial one in that it is clinically nondestructive.
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http://dx.doi.org/10.1016/j.jmbbm.2021.104593DOI Listing
September 2021

Effective and biocompatible antibacterial surfaces via facile synthesis and surface modification of peptide polymers.

Bioact Mater 2021 Dec 14;6(12):4531-4541. Epub 2021 May 14.

State Key Laboratory of Bioreactor Engineering, College of Chemistry, Chemical Engineering and Materials Science, East China University of Science and Technology, Shanghai, 200237, China.

It is an urgent need to tackle drug-resistance microbial infections that are associated with implantable biomedical devices. Host defense peptide-mimicking polymers have been actively explored in recent years to fight against drug-resistant microbes. Our recent report on lithium hexamethyldisilazide-initiated superfast polymerization on amino acid -carboxyanhydrides enables the quick synthesis of host defense peptide-mimicking peptide polymers. Here we reported a facile and cost-effective thermoplastic polyurethane (TPU) surface modification of peptide polymer (DLL: BLG = 90 : 10) using plasma surface activation and substitution reaction between thiol and bromide groups. The peptide polymer-modified TPU surfaces exhibited board-spectrum antibacterial property as well as effective contact-killing ability . Furthermore, the peptide polymer-modified TPU surfaces showed excellent biocompatibility, displaying no hemolysis and cytotoxicity. study using methicillin-resistant (MRSA) for subcutaneous implantation infectious model showed that peptide polymer-modified TPU surfaces revealed obvious suppression of infection and great histocompatibility, compared to bare TPU surfaces. We further explored the antimicrobial mechanism of the peptide polymer-modified TPU surfaces, which revealed a surface contact-killing mechanism by disrupting the bacterial membrane. These results demonstrated great potential of the peptide-modified TPU surfaces for practical application to combat bacterial infections that are associated with implantable materials and devices.
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http://dx.doi.org/10.1016/j.bioactmat.2021.05.008DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8138731PMC
December 2021

Smart fibers for energy conversion and storage.

Chem Soc Rev 2021 Jun;50(12):7009-7061

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Fibers have played a critical role in the long history of human development. They are the basic building blocks of textiles. Synthetic fibers not only make clothes stronger and more durable, but are also customizable and cheaper. The growth of miniature and wearable electronics has promoted the development of smart and multifunctional fibers. Particularly, the incorporation of functional semiconductors and electroactive materials in fibers has opened up the field of fiber electronics. The energy supply system is the key branch for fiber electronics. Herein, after a brief introduction on the history of smart and functional fibers, we review the current state of advanced functional fibers for their application in energy conversion and storage, focusing on nanogenerators, solar cells, supercapacitors and batteries. Subsequently, the importance of the integration of fiber-shaped energy conversion and storage devices via smart structure design is discussed. Finally, the challenges and future direction in this field are highlighted. Through this review, we hope to inspire scientists with different research backgrounds to enter this multi-disciplinary field to promote its prosperity and development and usher in a truly new era of smart fibers.
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http://dx.doi.org/10.1039/d0cs01603aDOI Listing
June 2021

High specific capacitance cotton fiber electrode enhanced with PPy and MXene by in situ hybrid polymerization.

Int J Biol Macromol 2021 Jun 20;181:1063-1071. Epub 2021 Apr 20.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, 2999 North Renmin Road, Shanghai 201620, China.

Fiber electrodes are the main functional elements of flexible and textile-based storage devices. This study proposes a Polypyrrole (PPy) and MXene composite, grown on cotton fiber, as a high capacitance electrode. Pyrrole (Py) and MXene are processed and deposited along with an in-situ polymerization. The mass and areal capacitance of the assembled (PPy/MXene)@Cotton electrode respectively reach to 506.6 F g, at current density of 1 A g and 455.9 mF cm at scan rate of 0.9 mA cm. These values outperform the [email protected] fiber electrode, around 45.8% and 119% respectively. As-prepared fiber electrodes with mechanical strength of 107.3 MPa and conductivity of 60.8 S/m, offer intriguing application prospects in the field of weaving and flexible fibrous supercapacitors.
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http://dx.doi.org/10.1016/j.ijbiomac.2021.04.112DOI Listing
June 2021

Ligament-Inspired Tough and Anisotropic Fibrous Gel Belt with Programed Shape Deformations Dynamic Stretching.

ACS Appl Mater Interfaces 2021 Apr 14;13(16):19291-19300. Epub 2021 Apr 14.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, 2999 North Renmin Road, Shanghai 201620, P. R. China.

Nature provides perpetual inspiration for exploring anisotropic materials to implement complex functions and motions like biological organisms. In particular, fibrous hydrogel-based anisotropic aggregates have attracted tremendous interest as fantastic materials for development into artificial ligaments or muscles. Such aggregates combine the structural anisotropy and macroscopic flexibility of fiber materials, with the intelligence, softness, and wetness of hydrogel materials. However, controlled fabrication of such hydrogels with aligned microstructures, even in a macroscopic level, remains a challenge. Here, a facile and general strategy was proposed to develop ligament-inspired multistructural (mono/bilayer) gel belts via dynamic stretching of multistrand pregels, accompanied by the simultaneous assembly of hydrogel fibers. The resultant gel belts evolved into anisotropic and aligned micro- and macrostructures, exhibiting high elastic moduli (0.01-23.5 MPa) and unique anisotropic swelling behaviors. Through further physical and chemical structure design, bioinspired multiple fibrous gel-based actuators were developed to achieve anisotropic, relatively fast (within 60 s), and delicate macroscopic shape deformations. This work provides a great platform for the design and construction of next-generation soft materials for biomimetic tissues.
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http://dx.doi.org/10.1021/acsami.1c02351DOI Listing
April 2021

Self-Perpetuating Carbon Foam Microwave Plasma Conversion of Hydrocarbon Wastes into Useful Fuels and Chemicals.

Environ Sci Technol 2021 05 6;55(9):6239-6247. Epub 2021 Apr 6.

Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.

White wastes (unseparated plastics, face masks, textiles, etc.) pose a serious challenge to sustainable human development and the ecosystem and have recently been exacerbated due to the surge in plastic usage and medical wastes from COVID-19. Current recycling methods such as chemical recycling, mechanical recycling, and incineration require either pre-sorting and washing or releasing CO. In this work, a carbon foam microwave plasma process is developed, utilizing plasma discharge to generate surface temperatures exceeding ∼3000 K in a N atmosphere, to convert unsorted white wastes into gases (H, CO, CH, CH, CH, etc.) and small amounts of inorganic minerals and solid carbon, which can be buried as artificial "coal". This process is self-perpetuating, as the new solid carbon asperities grafted onto the foam's surface actually increase the plasma discharge efficiency over time. This process has been characterized by optical probes and infrared sensors and optimized to handle most of the forms of white waste without the need for pre-sorting or washing. Thermal measurement and modeling show that in a flowing reactor, the device can achieve locally extremely high temperatures, but the container wall will still be cold and can be made with cheap materials, and thus, a miniaturized waste incinerator is possible that also takes advantage of intermittent renewable electricity.
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http://dx.doi.org/10.1021/acs.est.0c06977DOI Listing
May 2021

Improving the Physical-Mechanical Property of Dental Composites by Grafting Methacrylate-Polyhedral Oligomeric Silsesquioxane onto a Filler Surface.

ACS Biomater Sci Eng 2021 04 2;7(4):1428-1437. Epub 2021 Apr 2.

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

Endowing dental composites with excellent interfacial bonding through filler surface modification is pivotal to improve the physical-mechanical property and prolong the life of composite fillings. In this study, methacrylate-polyhedral oligomeric silsesquioxane (MA-POSS) acts as a "molecular bridge" between the commonly used SiO particles and the methacrylate-based resin matrix via a thiol-ene click reaction to construct MA-POSS/SiO (p-SiO) hybrid particles. Synthesized p-SiO exhibited the roughest surface morphology and had more polymerizable groups, in comparison with SiO and silanized SiO. Furthermore, the p-SiO particles were used as a reinforcement to fabricate bisphenol A glycerolate dimethacrylate/tri(ethyleneglycol) dimethacrylate-based dental composites, where the SiO- and silanized SiO-filled composites served as the control groups, and the filler loading was fixed at 65 wt %. Results of the mechanical properties indicated that the hybrid p-SiO particles significantly improved the flexural strength, flexural modulus, compressive strength, and work of fracture of dental composites, giving improvements of 251.2, 17.89, 122.3, and 1094%, respectively, over the SiO-filled composites due to the strong interfacial interaction between the resin matrix and p-SiO. Additionally, this optimal p-SiO-loaded composite also presented better polymerization shrinkage, acceptable degree of conversion, curing depth, and cell viability. Grafting of MA-POSS onto a filler surface is a promising filler surface modification to improve the resin matrix/filler interfacial interaction, leading to the enhanced overall performance of composites.
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http://dx.doi.org/10.1021/acsbiomaterials.1c00152DOI Listing
April 2021

A cascaded enzyme-loaded Fe-hemoporfin framework for synergistic sonodynamic-starvation therapy of tumors.

Nanoscale 2021 Mar 16;13(11):5910-5920. Epub 2021 Mar 16.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Enzyme-loaded nanosystems with multimodal therapeutic functions have received increasing attention in the treatment of malignant tumors. Herein, we designed and prepared cascaded dual-enzyme-augmented Fe-hemoporfin framework nanosonosensitizers for synergistic sonodynamic-starvation therapy of tumors. Amorphous Fe-hemoporfin frameworks (FeHF) with an average size of ∼85 nm were synthesized by assembling the clinical drug hemoporfin with Fe ions. Then, FeHF was used to load dual enzymes (glucose oxidase (GOx) and catalase (CAT)) and modified by PEGylated folic acid-conjugated lipids. The dual-enzyme loaded FeHF (FeHF-GOx/CAT) exhibited higher efficiency not only for glucose depletion but also for ultrasound (US)-triggered O generation than that of pure FeHF, resulting from the cascaded catalytic reaction from the dual-enzyme system. As observed by magnetic resonance imaging, the intravenously injected FeHF-GOx/CAT was accumulated within tumors. The FeHF-GOx/CAT + US exhibited the highest inhibition effect compared to the FeHF-CAT + US (only SDT) or FeHF-GOx/CAT (only starvation therapy), due to the synergistic effects of SDT and starvation therapy. Therefore, the cascaded dual-enzyme loading strategy can increase the SDT efficiency of FeHF, which may guide further works in the development of efficient nanosonosensitizers.
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http://dx.doi.org/10.1039/d0nr08508aDOI Listing
March 2021

Size-controllable synthesis of dendritic porous silica as reinforcing fillers for dental composites.

Dent Mater 2021 06 11;37(6):961-971. Epub 2021 Mar 11.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Material Science and Engineering, Donghua University, Shanghai 201620, PR China.

Objective: Porous materials, especially porous silica particles are of great interest in different areas, and have applied in dental composites as inorganic fillers, due to their potential in constructing micromechanical interlocking at the filler-resin matrix interfaces. However, the facile and precise synthesis of hierarchical porous silica with graded sizes is still a great challenge.

Methods: Here, we synthesized dendritic porous silica (DPS) with center-radial hierarchical pores and controllable size ranging from 75 to 1000nm by varying simultaneously the amounts of silica precursor and template in the microemulsion. A plausible nucleation-growth mechanism for the structural formation and the size tunability of the DPS particles was further put forward. These DPS particles were then formulated with Bis-GMA/TEGDMA resin.

Results: The particle size and morphology influenced the mechanical properties of dental composites. Particularly, DPS-500 particles (average size: 500nm) exhibited the superior reinforcing effect, giving large improvements of 32.0, 96.7, 51.9, and 225.6% for flexural strength (S), flexural modulus (E), compressive strength (S), and work of fracture (WOF), respectively, over the DPS-75 filled composite. All DPS filler sized exhibited similar degree of conversions and curing depths. Furthermore, the DPS-500 filled composite presented better cytocompatibility than commercial Z250 XT.

Significance: The facile synthesis of DPS particles developed here and the understanding of the influence of the filler size and morphology on the composite properties provide a shortcut to design porous silica with precise size control and dental composites with superior performance. These DPS particles could also have promising applications in biomedicine, catalysis, adsorption, and cancer therapy.
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http://dx.doi.org/10.1016/j.dental.2021.02.015DOI Listing
June 2021

Host-guest chemistry of giant molecular shape amphiphiles based on POSS-PDI conjugates.

Nanoscale 2021 Feb;13(7):4295-4300

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Center for Advanced Low-Dimension Materials, Donghua University, 201620, Shanghai, P. R. China.

Giant shape amphiphiles (GSA) are giant molecules made with nano-building blocks that have distinct shapes. The incompatible packing behaviors of the nano-building blocks of GSA could create cavities within certain conformers of the GSA, but the host-guest chemistry of GSA has not been explored yet. In this study, POSS-PDI-POSS (PPP), which is made by connecting two nano-cubes, isobutyl-polyhedral oligomeric silsesquioxanes (POSS), to a conjugated π-conjugated core, perylene diimide (PDI), is demonstrated as a novel acyclic synthetic host. In its bent conformer, PPP shows a cavity next to its PDI core. Via forming host-guest complexes with π-conjugated guests such as pyrene and perylene, PPP is found to transform from the bent-conformer into the extended-conformer, creating the steric features to accommodate guest molecules. Subsequent thermal annealing of the host-guest complexes removes the π-conjugated guests and restores the bent conformation and photophysical properties of PPP, which verifies that PPP, as a novel acyclic host, is capable of dynamic host-guest assembly. Moreover, the results prove that cavities at the molecular level can be created by connecting nano-building blocks with distinct shapes. This finding may inspire developments in the host-guest chemistry of GSA and nanomaterial innovation.
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http://dx.doi.org/10.1039/d0nr08934fDOI Listing
February 2021

Ultrasound-Mediated Remotely Controlled Nanovaccine Delivery for Tumor Vaccination and Individualized Cancer Immunotherapy.

Nano Lett 2021 02 1;21(3):1228-1237. Epub 2021 Feb 1.

Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, Jiangsu 215123, China.

Vaccines are one of utmost important weapons in modern medicine to fight a wide range of diseases. To achieve optimal vaccination effects, repeated injections of vaccines are often required, which would largely decrease patient comfort. Herein, an ultrasound-responsive self-healing hydrogel system loaded with nanovaccines is designed for remotely controlled tumor vaccine release and individualized cancer immunotherapy. The gel could be transformed into sol status in response to ultrasound treatment, allowing a burst release of nanovaccines, and self-healed to gel afterward. For mice with a single subcutaneous injection of nanovaccine-loaded gel and multiple ultrasound treatments, repeatedly released nanovaccines could elicit antitumor immune responses, which in combination with immune checkpoint blockade could effectively inhibit established tumors, and prevent postoperative tumor metastases and recurrence based on our personalized nanovaccine system. This work presents an easy-to-operate strategy to realize controllable and durable delivery of vaccines against cancer and potentially other types of diseases.
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http://dx.doi.org/10.1021/acs.nanolett.0c03646DOI Listing
February 2021

Effect of Storage Conditions on the Thermal Stability and Crystallization Behaviors of Poly(L-Lactide)/Poly(D-Lactide).

Polymers (Basel) 2021 Jan 12;13(2). Epub 2021 Jan 12.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, Shanghai 201620, China.

Polylactide (PLA) is a biodegradable thermoplastic aliphatic polyester. The thermal stability and crystallization behavior of PLA are extremely sensitive to storage, processing, and usage conditions. This work systematically studied the thermal stability and crystallization behavior of poly(L-lactide) (PLLA), poly(D-lactide) (PDLA), and a PLLA/PDLA (LD) blend, which were stored under two sets of laboratory storage conditions: (1) stored in a vacuum-free desiccator and (2) stored in vacuum-sealed bags. Both were stored at room temperature for 3 years. Gel permeation chromatography results revealed that the PLLA, PDLA, and LD samples hydrolyzed slowly when stored in vacuum-sealed bags and degraded significantly when stored in a vacuum-free desiccator; this process significantly reduced the thermal stability of the samples stored in the vacuum-free desiccator. Owing to hydrolysis, the levorotation and dextrorotation (L- and D-) molecular chains were shortened; consequently, more nuclei were formed, and this caused the melting points of the PLLA, PDLA, and LD samples to decrease and the melting enthalpy of the crystals in these samples to increase. Wide-angle X-ray diffraction analysis revealed that when the L- and D- molecular chains were packed side by side to form stereocomplex crystals and the randomly arranged L- and D- molecular chains were easy hydrolyzed and degraded, this interfered with the formation of homocrystals in LD. When PLLA, PDLA, and LD samples are stored in a vacuum-free desiccator, they will be significantly hydrolyzed, resulting in the formation of only stereocomplex crystals, and no homocrystals are observed.
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http://dx.doi.org/10.3390/polym13020238DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7828138PMC
January 2021

Trap Distribution and Conductivity Synergic Optimization of High-Performance Triboelectric Nanogenerators for Self-Powered Devices.

ACS Appl Mater Interfaces 2021 Jan 7;13(2):2566-2575. Epub 2021 Jan 7.

State Key Laboratory for Modification of Chemical Fibers & Polymer Materials, College of Materials Science & Engineering, Donghua University, Shanghai 201620, P. R. China.

Exploring effective methods of increasing the triboelectric charge density of tribo-materials to boost the output performance of triboelectric nanogenerators (TENGs) is crucial for expanding their practical applicability in modern smart devices. This study discusses the incorporation of various polymeric dielectric layers between the tribo-material and electrode components of TENGs, which improved their electrical output performance to varying degrees. The TENG demonstrating the largest improvement (1200 V) was obtained after adding a polyimide layer. The analysis presented herein suggests that incorporating a dielectric layer with high trap energy means that more charges are held in deep traps; thus, such TENGs demonstrate the best electrical performance. Additionally, when a dielectric layer is added to the triboelectric material, the enhanced TENG output is related to the volume conductivity of the triboelectric material, but not to its electronegativity or surface structure. Finally, the optimized TENG developed in this work demonstrates energy harvesting capabilities and can function as a self-powered sensor applied in an intelligent housing system and as an emergency fall detection/alert system for the elderly and the sick.
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http://dx.doi.org/10.1021/acsami.0c18243DOI Listing
January 2021

Thermal Stability of Bio-Based Aliphatic-Semiaromatic Copolyester for Melt-Spun Fibers with Excellent Mechanical Properties.

Macromol Rapid Commun 2021 Feb 18;42(3):e2000498. Epub 2020 Dec 18.

College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China.

Flexible aliphatic poly(lactic acid) is introduced into polyethylene terephthalate through copolymerization to prepare biodegradable copolyester, which aims to solve the non-degradability of polyethylene terephthalate (PET) and realize the greening of raw materials. In this work, poly(ethylene terephthalate-co-lactic acid) random copolyesters (PETLAs) of lactic acid composition from 10 to 50% is synthesized via one-pot method. The chemical structure and composition, thermal property, and crystallization property of prepared PETLAs resin are characterized. The results shows that the introduction of LA segment forms random copolyester, and the flexible LA segment results in slight decrease in the glass transition temperatures (T ), melting point (T ), and crystallinity (X ) of the copolyesters. The thermal stability of PETLAs is better, and the initial decomposition temperature of PETLA-10 can reach 394 °C. The PETLAs resin exhibits good processability, and PETLAs fibers are prepared by melt spinning. The strength of PETLA-10 fiber can reach 260 MPa after drawing treatment, and the elongation at break can reach 130%. Taking advantage of their features, PETLAs as an innovative bio-based polymer are expected to achieve ecofriendly applications in the fields of fiber, plastic, and film.
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http://dx.doi.org/10.1002/marc.202000498DOI Listing
February 2021

Functional fillers for dental resin composites.

Acta Biomater 2021 03 5;122:50-65. Epub 2020 Dec 5.

Département de Chimie, Université de Montréal, C.P. 6128, Succursale Centre-ville, Montréal, Québec, H3C 3J7, Canada. Electronic address:

Dental resin composites (DRCs) are popular materials to repair caries. Although various types of DRCs with different characteristics have been developed, restoration failures still exist. Bulk fracture and secondary caries have been considered as main causes for the failure of composites restoration. To address these problems, various fillers with specific functions have been introduced and studied. Some fillers with specific morphologies such as whisker, fiber, and nanotube, have been used to increase the mechanical properties of DRCs, and other fillers releasing ions such as Ag, Ca, and F, have been used to inhibit the secondary caries. These functional fillers are helpful to improve the performances and lifespan of DRCs. In this article, we firstly introduce the composition and development of DRCs, then review and discuss the functional fillers classified according to their roles in the DRCs, finally give a summary on the current research and predict the trend of future development.
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http://dx.doi.org/10.1016/j.actbio.2020.12.001DOI Listing
March 2021

Enantiomeric Switching of the Circularly Polarized Luminescence Processes in a Hierarchical Biomimetic System by Film Tilting.

ACS Nano 2021 01 4;15(1):1397-1406. Epub 2020 Dec 4.

Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, Institute for Advanced Study and Development of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong, China.

Circularly polarized luminescence (CPL) switching has attracted great attention due to the potential applications in chiral photonics and electronics. However, the lack of examples to achieve switchable CPL within a single material in the dry solid state hampers the scope of applications. Herein, we demonstrate a crystalline chiral polymer film as a polarizing medium consisting of radially assembled twisted crystallites, where achiral aggregation-induced emissive luminogens (AIEgens) are confined between the twisted crystalline stacks, eventually yielding handedness-switchable CPL by simple film tilting. Hierarchically organized twisted crystallites create the selective reflection activity of the polarizing medium. Upon film tilting, enantiomeric switching is realized by selectively collecting transmitted and reflected CPL components. The confined AIEgens in the crystalline polarizing system show a great enhancement of the luminescence efficiency. Moreover, the approach is general with broadband activity, and various AIEgens could be applied to generate full-color-tunable CPL. Additionally, the rigid and continuous nature of this polarizing system affords enhanced optical stability and facile modulation, developing a general route for designing chiroptical materials.
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http://dx.doi.org/10.1021/acsnano.0c08665DOI Listing
January 2021

One Responsive Stone, Three Birds: Mn(III)-Hemoporfin Frameworks with Glutathione-Enhanced Degradation, MRI, and Sonodynamic Therapy.

Adv Healthc Mater 2021 02 4;10(3):e2001463. Epub 2020 Dec 4.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, China.

Ultrasound-driven sonodynamic therapy (SDT) catches numerous attentions for destroying deep-seated tumors, but its applications suffer from unsatisfactory therapeutic effects and metabolism. Furthermore, SDT is usually weakened by the complex tumor microenvironment, such as the overexpression of glutathione (GSH). To address these issues, Mn(III)-hemoporfin frameworks (Mn(III)-HFs) are reported as nanosonosensitizers by using biocompatible hematoporphyrin monomethyl-ether (HMME) to coordinate with Mn(III) ions. Mn(III)-HFs/PEG can react with GSH to produce Mn(II) ions and oxidized glutathione (GSSG), resulting in three fascinating features: 1) the redox reaction facilitates the decomposition of Mn(III)-HFs/PEG and then collapse of nanostructures, improving the biodegradability; 2) Mn(II) ions with five unpaired 3d-electrons exhibit better magnetic resonance imaging (MRI) ability compared to Mn(III) ions with four electrons; 3) both the depletion of endogenous GSH and the dissociated HMME boost O generation ability under US irradiation. As a result, when Mn(III)-HFs/PEG dispersion is intravenously administered into mice, it exhibits high-contrast T /T dual-modal MRI and significant suppression for the growth rate of the deep-seated tumor. Furthermore, Mn(III)-HFs/PEG can be efficiently metabolized from the mice. Therefore, Mn(III)-HFs/PEG exhibit GSH-enhanced degradation, MRI, and SDT effects, which provide some insights on the developments of other responsive nanosonosensitizers.
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http://dx.doi.org/10.1002/adhm.202001463DOI Listing
February 2021

Fast Heat Transport Inside Lithium-Sulfur Batteries Promotes Their Safety and Electrochemical Performance.

iScience 2020 Oct 18;23(10):101576. Epub 2020 Sep 18.

State Key Lab for Modification of Chemical Fibers & Polymer Materials, College of Materials Science & Engineering, Donghua University, Shanghai 201620, China.

Lithium-sulfur batteries are paid much attention owing to their high specific capacity and energy density. However, their practical applications are impeded by poor electrochemical performance due to the dissolved polysulfides. The concentration of soluble polysulfides has a linear relationship with the internal heat generation. The issue of heat transport inside lithium-sulfur batteries is often overlooked. Here, we designed a functional separator that not only had a high thermal conductivity of 0.65 W m K but also alleviated the diffusion of dissolved active materials to the lithium anode, improving the electrochemical performance and safety issue. Lithium-sulfur batteries with the functional separator have a specific capacity of 1,126.4 mAh g at 0.2 C, and the specific capacity can be remained up to 893.5 mAh g after 100 cycles. Pouch Cells with high sulfur loading also showed a good electrochemical performance under a lean electrolyte condition of electrolyte/sulfur (E/S) = 3 μL mg.
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http://dx.doi.org/10.1016/j.isci.2020.101576DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7549117PMC
October 2020

Graphene-Like Carbon Film Wrapped Tin (II) Sulfide Nanosheet Arrays on Porous Carbon Fibers with Enhanced Electrochemical Kinetics as High-Performance Li and Na Ion Battery Anodes.

Adv Sci (Weinh) 2020 Sep 20;7(18):1903045. Epub 2020 Aug 20.

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

SnS, is a promising anode material for lithium ion batteries (LIBs) and sodium ion batteries (SIBs), however, undergoes poor cyclic lifespan due to its huge volume changes and bad electroconductivity. Here, a modified CVD method is used to directly grow graphene-like carbon film on the surface of SnS nanosheet arrays which are supported by Co-, N-modified porous carbon fibers ([email protected]@G). In the strategy, the SnS nanosheet arrays confined into the integrated carbon matrix containing porous carbon fibers and graphene-like carbon film, perform a greatly improved electrochemical performance. In situ TEM experiments reveal that the vertical graphene-like carbon film can not only protect the SnS nanosheet from destruction well and enhance the conductivity, but also transforms SnS nanosheet into ultrafine nanoparticles to promote the electrochemical kinetics. Systematic electrochemical investigations exhibit that the [email protected]@G electrode delivers a stable reversible capacity of 529 mAh g at a high current density of 5 A g for LIBs and 541.4 mAh g at 2 A g for SIBs, suggesting its good potential for anode electrodes.
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http://dx.doi.org/10.1002/advs.201903045DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7509643PMC
September 2020

Integrated dynamic wet spinning of core-sheath hydrogel fibers for optical-to-brain/tissue communications.

Natl Sci Rev 2021 Sep 31;8(9):nwaa209. Epub 2020 Aug 31.

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.

Hydrogel optical light-guides have received substantial interest for applications such as deep-tissue biosensors, optogenetic stimulation and photomedicine due to their biocompatibility, (micro)structure control and tissue-like Young's modulus. However, despite recent developments, large-scale fabrication with a continuous synthetic methodology, which could produce core-sheath hydrogel fibers with the desired optical and mechanical properties suitable for deep-tissue applications, has yet to be achieved. In this study, we report a versatile concept of integrated light-triggered dynamic wet spinning capable of continuously producing core-sheath hydrogel optical fibers with tunable fiber diameters, and mechanical and optical propagation properties. Furthermore, this concept also exhibited versatility for various kinds of core-sheath functional fibers. The wet spinning synthetic procedure and fabrication process were optimized with the rational design of the core/sheath material interface compatibility [core = poly(ethylene glycol diacrylate--acrylamide); sheath = Ca-alginate], optical transparency, refractive index and spinning solution viscosity. The resulting hydrogel optical fibers exhibited desirable low optical attenuation (0.18 ± 0.01 dB cm with 650 nm laser light), excellent biocompatibility and tissue-like Young's modulus (<2.60 MPa). The optical waveguide hydrogel fibers were successfully employed for deep-tissue cancer therapy and brain optogenetic stimulation, confirming that they could serve as an efficient versatile tool for diverse deep-tissue therapy and brain optogenetic applications.
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http://dx.doi.org/10.1093/nsr/nwaa209DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8433079PMC
September 2021
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