Well-defined and biocompatible hydrogels with toughening and reversible photoresponsive properties.

In the present study, novel hydrogels with extremely high strength, reversible photoresponsive and excellent biocompatible properties were prepared. The functional hydrogels were synthesized from a well-defined poly (ethylene glycol) polymer with spiropyran groups at a given position (PEG-SP) via a Cu(i)-catalyst Azide-Alkyne Cycloaddition (CuAAC) reaction. The molecular structures of the sequential intermediates for PEG-SP hydrogel preparation were verified by (1)HNMR and FT-IR. The mechanical property, swelling ratio, compression strength, surface hydrophilicity, and biocompatibility of the resulting hydrogel were characterized. Since spiropyran is pivotal to the switch in hydrophilicity on the hydrogel surface, the swelling ratio of PEG-SP hydrogel under Vis irradiation has a major decrease (155%). Before and after UV light irradiation, the contact angle of the hydrogel has a change of 13.8°. The photoresponsive property of this hydrogel was thus demonstrated, and such a property was also shown to be reversible. The well-defined PEG-SP hydrogel can also sustain a compressive stress of 49.8 MPa without any macro- or micro-damage, indicating its outstanding mechanical performance. Furthermore, it possessed excellent biocompatibility as demonstrated by its performance in an in vivo porcine subcutaneous implantation environment. No inflammation was observed and it got along well with the adjacent tissue. The above features indicate that PEG-SP hydrogels are promising as an implantable matrix for potential applications in biomaterial.

Multifunctional, Degradable Wearable Sensors Prepared with an Initiator and Crosslinker-Free Method.

The present zwitterionic hydrogel-based wearable sensor exhibits various limitations, such as limited degradation capacity, unavoidable toxicity resulting from initiators, and poor mechanical properties that cannot satisfy practical demands. Herein, we present an initiator and crosslinker-free approach to prepare polyethylene glycol (PEG)@poly[2-(methacryloyloxy)ethyl] dimethyl-(3-sulfopropyl) (PSBMA) interpenetrating polymer network (IPN) hydrogels that are self-polymerized via sunlight-induced and non-covalent crosslinking through electrostatic interaction and hydrogen bonding among polymer chains. The PEG@PSBMA IPN hydrogel possesses tissue-like softness, superior stretchability (∼2344.6% elongation), enhanced fracture strength (∼39.5 kPa), excellent biocompatibility, antibacterial property, reliable adhesion, and ionic conductivity. Furthermore, the sensor based on the IPN hydrogel demonstrates good sensitivity and cyclic stability, enabling effective real-time monitoring of human body activities. Moreover, it is worth noting that the excellent degradability in the saline solution within 8 h makes the prepared hydrogel-based wearable sensor free from the electronic device contamination. We believe that the proposed strategy for preparing physical zwitterionic hydrogels will pave the way for fabricating eco-friendly wearable devices.

Preparation of fluorescent organometallic porphyrin complex nanogels of controlled molecular structure via reverse-emulsion click chemistry.

Here, we are the first to report a novel approach to preparing well-defined poly(ethylene glycol) (PEG) fluorescent nanogels, with well-defined molecular structures and desired functionalities via reverse (mini)emulsion copper(I)-catalyzed azide-alkyne cycloaddition (REM-CuAAC). Nanogels with hydroxyl groups and Ga-porphyrin complex (Ga-porphyrin-OH nanogels), as well as with Ga-porphyrin complex and folate functional groups (Ga-porphyrin-FA), are successfully prepared. Nanogels of 30 and 120 nm in diameter are obtained and they exhibit an emission maxima within the wavelength range 700-800 nm. The nanogels could find uses in near infrared (NIR) imaging attributable to their fluorescence and their functionality for cell affinity.

Development of oxidized hydroxyethyl cellulose-based hydrogel enabling unique mechanical, transparent and photochromic properties for contact lenses.

With the development of smart devices, higher requirements are put forward for the stimuli-responsive materials. Stimuli-hydrogels as one kind of stimuli-responsive materials with hydrophilicity, demonstrate huge potential in developing intelligent devices for biomedical application. On this basis, we herein report that a sample method was devised to develop a novel composite hydrogel mainly based on oxidized hydroxyethyl cellulose and allyl co-polymer. Subsequently, a series of tests toward this oxidized hydroxyethyl cellulose-based hydrogel due to its structure and performance was applied. Here, the oxidized hydroxyethyl cellulose molecular chains were used as biomacromolecule templates to form Schiff base, borate and hydrogen bonds to obtain unique mechanical properties (fast recovery with almost no-hysteresis and remarkable compressive capacity), while a double bond functionalized spirooxazine (allyl spirooxazine derivative) was applied to endow photo- and pH sensitivity to the oxidized hydroxyethyl cellulose-based transparent hydrogel (T% = 93%) substrate. Furthermore, the oxidized hydroxyethyl cellulose-based hydrogel did exhibit good pH environment adaptability and noncytotoxicity in vitro test. Based on the advanced characteristics, the designed oxidized hydroxyethyl cellulose-based hydrogel has potential applications prospect in the development of safe, fashionable and pH- detectable contact lenses, thereby providing a new strategy for the development of smart, stylish contact lenses.

Nature-inspired chemistry toward hierarchical superhydrophobic, antibacterial and biocompatible nanofibrous membranes for effective UV-shielding, self-cleaning and oil-water separation.

Fabrication of environmental-friendly, low-cost, and free-standing superhydrophobic nanofibrous membranes with additional functionalities such as self-cleaning and UV-shielding properties is highly demanded for oil-water separation. Herein, we describe the preparation of multifunctional superhydrophobic nanofibrous membrane by using a facile and novel nature-inspired method, i.e., plant polyphenol (tannic acid) metal complex is introduced to generate rough hierarchical structures on the surface of an electrospun polyimide (PI) nanofibrous membrane, followed by modification of poly (dimethylsiloxane) (PDMS). Taking an as-prepared tannic acid - Al3+-based superhydrophobic membrane as an example, it not only exhibits anti-impact, low-adhesive and self-cleaning functions, but also presents excellent performance in the separation of various oil-water mixtures. A high flux up to 6935 l m-2 h-1 with a separation efficiency of over 99% and the oil contents in water below 5 ppm is obtained even after repeating use for twenty separation cycles. Additionally, the membrane exhibits excellent UV-shielding property, attributing to the inherent UV-absorbing ability of tannic acid. Furthermore, the membrane also possesses additional properties including antibacterial activity, good biocompatibility, robust mechanical strength, and excellent resistance to various harsh conditions. These attractive properties of the as-prepared membrane make it a promising candidate for potential applications in industrial oil-contaminated water treatments and oil-water separation.

Facile and cost-effective synthesis of glycogen-based conductive hydrogels with extremely flexible, excellent self-healing and tunable mechanical properties.

In materials science and engineering, the designing of hydrogels with excellent self-healing and tunable mechanical properties is an inviting issue. In this study, we introduce the sacrificial bonds interactions in a hybrid hydrogel of natural and synthetic polymers, to give a hydrogel with autonomous self-healing ability and tunable mechanical properties. Glycogen, a natural polymer tends to strengthen the hydrogel while PVA, a synthetic polymer plays a critical role in the flexibility and stretchability of the hydrogel. Hydrogels were designed by the sacrificial non-covalent interactions with physical cross-linking of the polymer chains to the trivalent metal ions. Functional groups of the polymers interact with sacrificial hydrogen bonds with and with the metal ions, they interact through sacrificial coordination interactions with different strength, results tunable sacrificial bonds. Weaker sacrificial bonds rupture prior to the strong sacrificial bonds upon external loading, which dissipate the energy and endow the hydrogel with adjustable mechanical and self-healing properties. The tunable mechanical properties and excellent self-healing efficiency enlarge the application areas of the developed hydrogel in various fields.

Preparation and applications of functional nanofibers based on the combination of electrospinning, controlled radical polymerization and 'Click Chemistry'.

This feature article provides an overview of the preparation of functional nanofibers by combined electrospinning, controlled radical polymerization and 'Click Chemistry'. A combination of the powerful capability of controlled radical polymerization and 'Click Chemistry' for the synthesis of functional macromolecules and on surface modification as well as their wide applicability to electrospinning materials, functional nanofibers with a crosslinked structure, core-shell structures, and switchable surface properties etc. were prepared. In addition, the applications of the functional nanofibers in antibacterial fields and controlled release are also explored.

Functional polymeric nanofibers from electrospinning.

Electrospinning has been recognized as a feasible process for fabrication of continuous fibers with diameters ranging from several micrometers down to a few nanometers. This article presents an overview of recent progress in functional polymeric nanofibers prepared by electrospinning. Except of functional nanofibers fabricated from electrospinning of functional polymers, nanofibers from a combined technology such as coaxial electrospinning, electrospinning with living radical polymerization, and electrospinning with surface modification, would also be introduced in this review. Furthermore, the functionality and application of nanofibers would also be highlighted.