Ambient Pressure Drying of Freeze-Cast Ceramics from Aqueous Suspension.

Freeze-casting has been wildly exploited to construct porous ceramics but usually requires costly and demanding freeze-drying (high vacuum, size limit, and supercooled chamber), which can be avoided by the ambient pressure drying (APD) technique. However, applying APD to freeze-cast ceramic based on an aqueous suspension is still challenging due to inert surface chemistry. Herein, a modified APD strategy is developed to improve the drying process of freeze-cast ceramics by exploiting the simultaneous ice etching, ionic cross-linking, and solvent exchange under mild conditions (-10-0 °C, ambient pressure). This versatile strategy is applicable to various ceramic species, metal ions, and freezing techniques. The incorporated metal ions not only enhance liquid-phase sintering, producing ceramics with higher density and mechanical properties than freeze-cast counterparts, but also render customizable coloration and antibacterial property. The cost-/time-efficient APD is promising for mass production and even successive production of large-size freeze-cast ceramics that exceed the size of commercial freeze-dryers.

A Magneto-Heated Silk Fibroin Scaffold for Anti-Biofouling Solar Steam Generation.

Macroscopic 3D porous materials are ideal solar evaporators for water purification. However, the limited sunlight intensity and penetrating depth during solar-driven evaporation cannot prevent the biofouling formation by photothermal effect, thus leading to the deterioration of evaporation rate. Herein, a magnetic heating strategy is reported for anti-biofouling solar steam generation based on a magnetic silk fibroin (SF) scaffold with bi-heating property. Under one sun, the solar-heated top surface of magnetic SF scaffolds accelerates water evaporation at 2.03 kg m-2 h-1 , while the unheated inner channels suffer from the formation of biofilm. When exposed to alternating magnetic field (AMF), the magnetic SF scaffold can be integrally heated, leading to an efficient inner temperature to prevent biofouling in channels for water transportation. Accordingly, magneto-heated scaffolds show steady water evaporation rates after exposure to S. aureus and E. coli, which maintained 93.6-94.6% of original performance. In contrast, the evaporation rates of the scaffolds without AMF treatment are reduced to 1.31 (S. aureus) and 1.32 (E. coli) kg m-2 h-1 , decreased by 35.5% and 35.0%, respectively. In addition, the magneto-heated scaffold inhibits biofouling formation in natural lake water, maintaining 99.5% original performance.

Oak-inspired anti-biofouling shape-memory unidirectional scaffolds with stable solar water evaporation performance.

Biomimetic porous materials have contributed to the enhancement of solar-driven evaporation rate in interfacial desalination and clean water production. However, due to the presence of numerous microbes in water environment, biofouling should occur inside porous materials to clog the channels for water transfer, resulting in obvious inhibition of the solar-driven evaporation efficacy in long-term use. To prevent and control biofouling in porous materials for solar-driven evaporation, a facile and environment-friendly design is required in real application. Oak wood possesses vertically aligned channels for transpiration and polyphenol compounds with antimicrobial activity. In this work, inspired by the oak wood, we developed an anti-biofouling shape-memory chitosan scaffold with unidirectional channels and tannic acid coating (oak-inspired scaffold). The shape-memory property facilitated rapid decoration with oak-inspired photothermal and anti-biofouling coating inside the scaffold, respectively, which also promotes the material durability by avoiding the external force-induced permanent structure failure. More importantly, the oak-inspired tannic acid coating not only prevented bacterial adhesion and colonization, but also inhibited fungal interference. They were subjected to a microbe-rich environment, and after 3 days, the evaporation rates of the untreated chitosan scaffolds were obviously decreased to 1.24, 1.16 and 1.19 kg m-2 h-1 for C. albicans, S. aureus and E. coli, respectively, which were only 65.6, 61.4 and 63.0% of original performance (1.89 kg m-2 h-1). In comparison, the oak-inspired scaffold exhibited a high solar-driven water evaporation rate after incubation in microbial suspensions (1.80, 1.70 and 1.75 kg m-2 h-1 for C. albicans, S. aureus and E. coli after 3 days) and lake water (1.74 kg m-2 h-1 after one month). The bioinspired anti-biofouling scaffolds maintain as high as 86.7-91.8% of the solar-driven water evaporation ability after exposure to a microbe-rich environment, which is conducive to develop a biomimetic long-term durable structure in water treatment.

Injectable ferrimagnetic silk fibroin hydrogel for magnetic hyperthermia ablation of deep tumor.

Due to the well-recognized biocompatibility, silk fibroin hydrogels have been developed for biomedical applications including bone regeneration, drug delivery and cancer therapy. For the treatment of cancer, silk-based photothermal agents exhibit the high photothermal conversion efficiency, but the limited light penetration depth of photothermal therapy restricts the treatment of some tumors in deep positions, such as liver tumor and glioma. To provide an alternative strategy, here we developed an injectable magnetic hydrogel based on silk fibroin and iron oxide nanocubes (IONCs). The as-prepared ferrimagnetic silk fibroin hydrogel could be easily injected through a syringe into tumor, especially rabbit hepatocellular carcinoma in deeper positions using ultrasound-guided interventional treatment. Compared with photothermal agents, the embedded IONCs endowed the ferrimagnetic silk fibroin hydrogel with remote hyperthermia performance under an alternating magnetic field, resulting in the effective magnetic hyperthermia of deep tumors including subcutaneously implanted tumor model in Balb/c mouse after the coverage of a fresh pork tissue and orthotopic transplantation liver tumor in rabbit. Furthermore, due to the confinement of IONCs in silk fibroin hydrogel, the undesired thermal damage toward normal tissue could be avoided compared with directly administrating monodispersed magnetic nanoparticles.

Enzyme-Responsive Ag Nanoparticle Assemblies in Targeting Antibacterial against Methicillin-Resistant Staphylococcus Aureus.

The abuse of antibiotics resulted in the emergence of antibiotics-resistant bacteria, which has raised a great social concern together with the impetus to develop effective antibacterial materials. Herein, the synthesis of biocompatible enzyme-responsive Ag nanoparticle assemblies (ANAs) and their application in the high-efficiency targeted antimicrobial treatment of methicillin-resistant Staphylococcus aureus (MRSA) have been demonstrated. The ANAs could collapse and undergo stable/collapsed transition on approaching MRSA because of the serine protease-like B enzyme proteins (SplB)-triggered decomposition of the branched copolymers which have been employed as the macrotemplate in the synthesis of responsive ANAs. This transition contributed greatly to the high targeting affinity and efficiency of ANAs to MRSA. The minimum inhibitory concentration and minimum bactericidal concentration against MRSA were 2.0 and 32.0 µg mL-1, respectively. Skin wound healing experiments confirmed that the responsive ANAs could serve as an effective wound dressing to accelerate the healing of MRSA infection.

Thermoresponsive in Situ Forming Hydrogel with Sol-Gel Irreversibility for Effective Methicillin-Resistant Staphylococcus aureus Infected Wound Healing.

An in situ forming hydrogel has emerged as a promising wound dressing recently. As physically cross-linked hydrogels are normally unstable, most in situ forming hydrogels are chemically cross-linked. However, big concerns have remained regarding the slow gelation and the potential toxicity of residual functional groups from cross-linkers or the polymer matrix. Herein, we report a sprayable in situ forming hydrogel composed of poly(N-isopropylacrylamide166-co-n-butyl acrylate9)-poly(ethylene glycol)-poly(N-isopropylacrylamide166-co-n-butyl acrylate9) copolymer (P(NIPAM166-co-nBA9)-PEG-P(NIPAM166-co-nBA9), denoted as PEP) and silver-nanoparticles-decorated reduced graphene oxide nanosheets (Ag@rGO, denoted as AG) in response to skin temperature. This thermoresponsive hydrogel exhibits intriguing sol-gel irreversibility at low temperatures for the stable dressing of a wound, which is attributed to the inorganic/polymeric dual network and abundant coordination interactions between Ag@rGO nanosheets and PNIPAM. The biocompatibility and antibacterial ability against methicillin-resistant Staphylococcus aureus (MRSA) of this PEP-AG hydrogel wound dressing are confirmed in vitro and in vivo, which could transparently promote the healing of a MRSA-infected skin defect.

Bioinspired Unidirectional Silk Fibroin-Silver Compound Nanowire Composite Scaffold via Interface-Mediated In Situ Synthesis.

Bioinspired unidirectional porous materials have emerged as a unique class of scaffolds for the fabrication of macroscopic nanomaterial assemblies. However, these scaffolds usually serve simply as mechanical carriers to support various building blocks. Here, we report that the unidirectional silk fibroin scaffold can not only act as a carrier, but also serve as a controllable multiscale reactor to achieve the in situ synthesis of a Ag3 PO4 nanowire network anchored to ordered channels. Both the silk fibroin matrix and the interface play important roles in the nucleation and growth of the Ag3 PO4 nanowires. This unidirectional composite scaffold can be used for efficient water disinfection. Furthermore, the facile chemical transformation of Ag3 PO4 in the composite scaffold into Ag2 S provided an analogous unidirectional composite silk scaffold that displays both efficient solar water evaporation effect and antibacterial activity. It is expected that this method can be extended to fabricate a series of silk-based unidirectional composite scaffolds with varying functionalities.

Liquid Exfoliation of Atomically Thin Antimony Selenide as an Efficient Two-Dimensional Antibacterial Nanoagent.

The ever-growing global crisis of multidrug-resistant bacteria has triggered a tumult of activity in the design and development of antibacterial formulations. Here, atomically thin antimony selenide nanosheets (Sb2Se3 NSs), a minimal-toxic and low-cost semiconductor material, were explored as a high-performance two-dimensional (2D) antibacterial nanoagent via a liquid exfoliation strategy integrating cryo-pretreatment and polyvinyl pyrrolidone (PVP)-assisted exfoliation. When cultured with bacteria, the obtained PVP-capped Sb2Se3 NSs exhibited intrinsic long-term antibacterial capability, probably due to the reactive oxygen species generation and sharp edge-induced membrane cutting during physical contact between bacteria and nanosheets. Upon near-infrared laser irradiation, Sb2Se3 NSs achieved short-time hyperthermia sterilization because of strong optical absorption and high photothermal conversion efficiency. By virtue of the synergistic effects of these two broad-spectrum antibacterial mechanisms, Sb2Se3 NSs exhibited high-efficiency inhibition of conventional Gram-negative Escherichia coli, Gram-positive methicillin-resistant Staphylococcus aureus, and wild bacteria from a natural water pool. Particularly, these three categories of bacteria were completely eradicated after being treated with Sb2Se3 NSs (300 µM) plus laser irradiation for only 5 min. In vivo wound healing experiment further demonstrated the high-performance antibacterial effect. In addition, Sb2Se3 NSs depicted excellent biocompatibility due to the biocompatible element constitute and bioinert PVP modification. This work enlightened that atomically thin Sb2Se3 NSs hold great promise as a broad-spectrum 2D antibacterial nanoagent for various pathogenic bacterial infections.

MnFe2O4 nanoparticles accelerate the clearance of mutant huntingtin selectively through ubiquitin-proteasome system.

Neurodegenerative disorders such as Huntington's disease (HD) are fundamentally caused by accumulation of misfolded aggregate-prone proteins. Previous investigations have shown that these toxic protein aggregates could be degraded through autophagy induced by small molecules as well as by nanomaterials. However, whether engineered nanomaterials have the capacity to degrade these protein aggregates via the ubiquitin-proteasome system (UPS), the other major pathway for intracellular protein turnover, was unknown. Herein, we have synthesized biocompatible MnFe2O4 nanoparticles (NPs) and demonstrated their unique effect in accelerating the clearance of mutant huntingtin (Htt) protein exhibiting 74 glutamine repeats [Htt(Q74)]. UPS, rather than autophagy, was responsible for the efficient Htt(Q74) degradation facilitated by MnFe2O4 NPs. Meanwhile, we demonstrated that MnFe2O4 NPs enhanced K48-linked ubiquitination of GFP-Htt(Q74). Moreover, ubiqinlin-1, but not p62/SQSTM1, served as the ubiquitin receptor that mediated the enhanced degradation of Htt(Q74) by MnFe2O4 NPs. Our findings may have implications for developing novel nanomedicine for the therapy of HD and other polyglutamine expansion diseases.

Nacre-mimic Reinforced Ag@reduced Graphene Oxide-Sodium Alginate Composite Film for Wound Healing.

With the emerging of drug-resistant bacterial and fungal pathogens, there raise the interest of utilizing versatile antimicrobial biomaterials to treat the acute wound. Herein, we report the spraying mediated assembly of a bio-inspired Ag@reduced graphene-sodium alginate (AGSA) composite film for effective wound healing. The obtained film displayed lamellar microstructures similar to the typical "brick-and-mortar" structure in nacre. In this nacre-mimic structure, there are abundant interfacial interactions between nanosheets and polymeric matrix, leading to remarkable reinforcement. As a result, the tensile strength, toughness and Young's modulus have been improved 2.8, 2.3 and 2.7 times compared with pure sodium alginate film, respectively. In the wound healing study, the AGSA film showed effective antimicrobial activities towards Pseudomonas aeruginosa, Escherichia coli and Candida albicans, demonstrating the ability of protecting wound from pathogenic microbial infections. Furthermore, in vivo experiments on rats suggested the effect of AGSA film in promoting the recovery of wound sites. According to MTT assays, heamolysis evaluation and in vivo toxicity assessment, the composite film could be applied as a bio-compatible material in vitro and in vivo. Results from this work indicated such AGSA film has promising performance for wound healing and suggested great potential for nacre-mimic biomaterials in tissue engineering applications.

Influence of Cu doping in borosilicate bioactive glass and the properties of its derived scaffolds.

Copper doped borosilicate glasses (BG-Cu) were studied by means of FT-IR, Raman, UV-vis and NMR spectroscopies to investigate the changes that appeared in the structure of borosilicate glass matrix by doping copper ions. Micro-fil and immunohistochemistry analysis were applied to study the angiogenesis of its derived scaffolds in vivo. Results indicated that the Cu ions significantly increased the B-O bond of BO4 groups at 980 cm(-1), while they decrease that of BO2O(-) groups at 1440-1470 cm(-1) as shown by Raman spectra. A negative shift was observed from (11)B and (29)Si NMR spectra. The (11)B NMR spectra exhibited a clear transformation from BO3 into BO4 groups, caused by the agglutination effect of the Cu ions and the charge balance of the agglomerate in the glass network, leading to a more stable glass network and lower ions release rate in the degradation process. Furthermore, the BG-Cu scaffolds significantly enhanced blood vessel formation in rat calvarial defects at 8 weeks post-implantation. Generally, it suggested that the introduction of Cu into borosilicate glass endowed glass and its derived scaffolds with good properties, and the cooperation of Cu with bioactive glass may pave a new way for tissue engineering.

A residue-free green synergistic antifungal nanotechnology for pesticide thiram by ZnO nanoparticles.

Here we reported a residue-free green nanotechnology which synergistically enhance the pesticides efficiency and successively eliminate its residue. We built up a composite antifungal system by a simple pre-treating and assembling procedure for investigating synergy. Investigations showed 0.25 g/L ZnO nanoparticles (NPs) with 0.01 g/L thiram could inhibit the fungal growth in a synergistic mode. More importantly, the 0.25 g/L ZnO NPs completely degraded 0.01 g/L thiram under simulated sunlight irradiation within 6 hours. It was demonstrated that the formation of ZnO-thiram antifungal system, electrostatic adsorption of ZnO NPs to fungi cells and the cellular internalization of ZnO-thiram composites played important roles in synergy. Oxidative stress test indicated ZnO-induced oxidative damage was enhanced by thiram that finally result in synergistic antifungal effect. By reducing the pesticides usage, this nanotechnology could control the plant disease economically, more significantly, the following photocatalytic degradation of pesticide greatly benefit the human social by avoiding negative influence of pesticide residue on public health and environment.

Selectively enhanced antibacterial effects and ultraviolet activation of antibiotics with ZnO nanorods against Escherichia coli.

In this paper, the selectively enhanced antibacterial effects of ZnO nanorods with several kinds of conventional medical antibiotics are investigated. Compares to gentamicin, clarithromycin and ofloxacin, ZnO nanorods could obviously achieve synergistic antibacterial effects with ceftriaxone against Escherichia coli (E. coli). Meanwhile, ultraviolet (UV) activation is adopted to induce higher antibacterial activity of ceftriaxone-ZnO nanorods than that of pure ceftriaxone or ZnO nanorods. The results of colony-forming capability test, infrared ray (IR) spectrum, and detection of reactive oxygen species (ROS) indicated that ceftriaxone may the facilitate the entry of ZnO nanorods into bacterial cell, and this effect would play an important role in mechanisms of such antibacterial behavior under the conditions of this study.