Thermo-responsive cascade antimicrobial platform for precise biofilm removal and enhanced wound healing.

Background: Bacterial infection, tissue hypoxia and inflammatory response can hinder infected wound repair. This study aimed to develop a multifunctional specific therapeutic photo-activated release nanosystem [HMPB@MB@AuNPs@PMB@HA (HMAPH)] by loading photosensitizer methylene blue (MB) into hollow mesoporous Prussian blue nanostructures and modifying the surface with gold particles, polymyxin B (PMB) and hydrophilic hyaluronic acid. Methods: The HMAPH was characterized using transmission electron microscopy, UV-vis, Fourier-transform infrared spectroscopy, X-ray diffraction and X-ray photon spectroscopy. The photothermal performance, iron ion release and free radical generation of the HMAPH were measured under different conditions to investigate its thermo-responsive cascade reaction. The antibacterial ability of HMAPH was investigated using live/dead fluorescence tests. The morphology and membrane integrity of Pseudomonas aeruginosa (P. aeruginosa) were investigated using transmission electron microscopy. The anti-biofilm activity of HMAPH was evaluated using crystal violet and SYBR Green I staining. Finally, we established a mouse model of a skin wound infected by P. aeruginosa to confirm the in vivo effectiveness of HMAPH. We used immunofluorescent staining, hematoxylin-eosin staining, Masson staining and enzyme-linked immunosorbent assay to examine whether HMAPH promoted wound healing and reduced inflammatory damage. Results: In this study, hyaluronic acid was decomposed under the action of hyaluronidase. Also, the exposed nanomaterials specifically bound to the outer membrane of P. aeruginosa through PMB to increase the membrane sensitivity to photodynamic treatment. Under dual-light irradiation, a large amount of iron ions released by HMAPH underwent a Fenton reaction with H2O2 in bacteria to generate hydroxyl radicals (•OH), enabling direct killing of cells by hyperthermia. Additionally, the photodynamic activity of MB released by photo-induced activation led to the generation of reactive oxygen species, achieving synergistic and effective inhibition of P. aeruginosa. HMAPH also inhibited biofilm formation and downregulated the expression of virulence factors. In vivo experiments revealed that HMAPH accelerated the healing of P. aeruginosa-infected wounds by promoting angiogenesis and skin regeneration, inhibiting the inflammatory response and promoting M1 to M2 polarization. Conclusions: Our study proposed a strategy against bacteria and biofilms through a synergistic photothermal-photodynamic-Fenton reaction, opening up new prospects for combating biofilm-associated infections.

In2S3@TiO2/In2S3 Z-Scheme Heterojunction with Synergistic Effect for Enhanced Photocathodic Protection of Steel.

In this work, a TiO2/In2S3 heterojunction film was successfully synthesized using a one-step hydrothermal method and applied in the photocathodic protection (PCP) of 304SS. The octahedral In2S3 and In2S3@TiO2 nanoparticles combined and coexisted with each other, with In2S3 quantum dots growing on the surface of TiO2 to form In2S3@TiO2 with a wrapping structure. The composite photoelectrode, which includes TiO2 with a mixed crystalline phase and In2S3, exhibited significantly enhanced PCP performance for 304SS compared with pure In2S3 and TiO2. The In2S3@TiO2/In2S3 composites with 0.3 g of P25 titanium dioxide (P25) showed the best protection performance, resulting in a cathodic shift of its OCP coupled with 304SS to -0.664 VAgCl. The electron transfer tracking results demonstrate that In2S3@TiO2/In2S3 forms a Z-scheme heterojunction structure. The enhanced PCP performance could be attributed to the synergistic effect of the mixed crystalline phase and the Z-scheme heterojunction system. The mixed crystalline phase of TiO2 provides more electrons, and these electrons are gathered at higher energy potentials in the Z-scheme system. Additionally, the built-in electric field further promotes the more effective electrons transfer from photoelectrode to the protected metals, thus, leading to enhanced photoelectrochemical cathodic protection of 304SS.

Integrated multifunctional nanoplatform for fluorescence detection and inactivation of Staphylococcus aureus.

Foodborne illness caused by Staphylococcus aureus (S. aureus) has posed a significant threat to human health. Herein, an integrated multifunctional nanoplatform was developed for fluorescence detection and inactivation of S. aureus based on cascade signal amplification coupled with single strand DNA-template copper nanoparticles (ssDNA-Cu NPs). Benefiting from reasonable design, one-step cascade signal amplification was achieved through strand displacement amplification combined with rolling circle amplification, followed by in-situ generation of copper nanoparticles. S. aureus detection could be performed through naked eye observation and microplate reader measurement of the red fluorescence signal. The multifunctional nanoplatform had satisfactory specificity and sensitivity, achieving 5.2 CFU mL-1 detection limit and successful detection of 7.3 CFU of S. aureus in spiked egg after < 5 h of enrichment. Moreover, ssDNA-Cu NPs could eliminate S. aureus to avoid secondary bacterial contamination without further treatment. Therefore, this multifunctional nanoplatform has potential application in food safety dtection.

An injectable multifunctional hydrogel for eradication of bacterial biofilms and wound healing.

Wound treatment is largely influenced by pre-existing hypoxic microenvironments and biofilms, which can severely diminish the efficacy of phototherapy, suggesting the importance of multifunctional nanoplatforms for synergistic treatment of wound infections. Here, we developed a multifunctional injectable hydrogel (PSPG hydrogel) by loading photothermal sensitive sodium nitroprusside (SNP) into Pt-modified porphyrin metal organic framework (PCN) and in situ modification of gold particles to form a near-infrared (NIR) light-triggered all-in-one phototherapeutic nanoplatform. The Pt-modified nanoplatform exhibits a remarkable catalase-like behavior and promotes the continuous decomposition of endogenous H2O2 into O2, thereby enhancing the photodynamic therapy (PDT) effect under hypoxia. Under dual NIR irradiation, PSPG hydrogel can not only produce hyperthermia (η=89.21%) but also generate reactive oxygen species and trigger NO release, contributing jointly to removal of biofilms and disruption of the cell membranes of methicillin-resistant Staphylococcus aureus (MRSA) and Escherichia coli (E. coli). In vivo experiments demonstrated a 99.9% reduction in bacterial burden on wounds. Additionally, PSPG hydrogel can accelerate MRSA-infected and Pseudomonas aeruginosa-infected (P. aeruginosa-infected) wound healing by promoting angiogenesis, collagen deposition, and suppressing inflammatory responses. Furthermore, in vitro and in vivo experiments revealed that PSPG hydrogel has good cytocompatibility. Overall, we proposed an antimicrobial strategy to eliminate bacteria through the synergistic effects of gas-photodynamic-photothermal killing, alleviating hypoxia in the bacterial infection microenvironment, and inhibiting biofilms, offering a new way against antimicrobial resistance and biofilm-associated infections. STATEMENT OF SIGNIFICANCE: The NIR light-triggered multifunctional injectable hydrogel nanoplatform (PSPG hydrogel) based on Pt-decorated gold nanoparticles with sodium nitroprusside (SNP)-loading porphyrin metal organic framework (PCN) as inner templates can efficiently perform photothermal conversion (η=89.21%) to trigger NO release from SNP, while continuously regulating the hypoxic microenvironment at the bacterial infection site through Pt-induced self-oxygenation, achieving efficient sterilization and removal of biofilm by synergistic PDT and PTT phototherapy. In vivo and in vitro experiments demonstrated that the PSPG hydrogel has significant anti-biofilm, antibacterial, and inflammatory regulatory functions. This study proposed an antimicrobial strategy to eliminate bacteria through the synergistic effects of gas-photodynamic-photothermal killing, alleviating hypoxia in the bacterial infection microenvironment, and inhibiting biofilms.

Van-mediated self-aggregating photothermal agents combined with multifunctional magnetic nickel oxide nanoparticles for precise elimination of bacterial infections.

Building a novel and efficient photothermal antibacterial nanoplatform is a promising strategy for precise bacterial elimination. Herein, a nanocomposite NiO NPs@AuNPs@Van (NAV) for selective MRSA removal was constructed by electrostatic self-assembly of highly photothermal magnetic NiO NPs and vancomycin (Van)-modified gold nanoparticles (AuNPs). In the presence of MRSA and under NIR irradiation, Van-mediated AuNPs can self-aggregate on MRSA surface, generating photothermal effect in situ and killing 99.6% MRSA in conjunction with magnetic NiO NPs. Additionally, the photothermal efficiency can be improved by magnetic enrichment due to the excellent magnetism of NAV, thereby enhancing the bactericidal effect at a lower experimental dose. In vitro antibacterial experiments and full-thickness skin wound healing test demonstrated that this combination therapy could effectively accelerate wound healing in MRSA-infected mice, increase collagen coverage, reduce IL-6 and TNF-α content, and upregulate VEGF expression. Biological safety experiments confirmed that NAV has good biocompatibility in vivo and in vitro. Overall, this work reveals a new type of nanocomposite with enhanced photothermal antibacterial activity as a potential nano-antibacterial agent for treating bacteria-infected wounds.

Ni Nanocrystals Supported on Graphene Oxide: Antibacterial Agents for Synergistic Treatment of Bacterial Infections.

The effects of antibiotics on bacterial infections are gradually weakened, leading to the wide development of nanoparticle-based antibacterial agents with unique physical and chemical properties and antibacterial mechanisms different from antibiotics. In this study, we fabricated the uniform and stable graphene oxide (GO)/Ni colloidal nanocrystal cluster (NCNC) nanocomposite by electrostatic self-assembly and investigated its synergistic antibacterial activity against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) in vitro. The GO/NCNC nanocomposite was shown to possess higher inhibition efficiency than a pure NCNC or GO suspension, with 99.5 and 100% inhibition against S. aureus and E. coli at a 125 µg/mL concentration, respectively. Antibacterial mechanism analysis revealed that (i) NCNCs decorated on GO can further enhance the antibacterial properties of GO by binding and capturing bacteria, (ii) the leaching of Ni2+ was detected during the interaction of GO/NCNCs and bacteria, resulting in a decrease in the number of bacteria, and (iii) the GO/NCNC nanocomposite can synergistically destroy the bacterial membrane through physical action and induce the reactive oxygen species generation, so as to further damage the cell membrane and affect ATPase, leakage of intercellular contents, and ultimately bacterial growth inhibition. Meanwhile, cell culture experiments demonstrated no adverse effect of GO/NCNCs on cell growth. These preliminary results indicate the high antibacterial efficiency of the GO/NCNC nanocomposite, suggesting the possibility to develop it into an effective antibacterial agent in the future against bacterial infections.

NIR-activated multi-hit therapeutic Ag2S quantum dot-based hydrogel for healing of bacteria-infected wounds.

Hydrogel dressings are highly biocompatible and can maintain a moist wound environment, suggesting constructing an efficient multi-modal antibacterial hydrogel platform is a promising strategy for treating bacterial wound infections. In this work, a composite Ag2S quantum dot/mSiO2 NPs hydrogel (NP hydrogel) with antibacterial ability was constructed by incorporating Ag2S quantum dots (QDs) modified by mesoporous silica (mSiO2) into the network structure of 3-(trimethoxylmethosilyl) propyl methacrylate based on free radical polymerization. The NP hydrogel showed outstanding controllable photothermal and photodynamic characteristics under 808 nm near infrared (NIR) light irradiation, with a photothermal conversion efficiency of 57.3%. Additionally, the release of Ag+ could be controlled by the inherent volume change of the NP hydrogel made of N-isopropylacrylamide (NIPAAm) and acrylamide (AAm) during NIR laser exposure, with the embedded Ag2S QDs working as a reservoir to release Ag+ continuously from the hydrogel matrix to achieve bactericidal activity. The synergetic effects between hyperthermia, radical oxygen species, and Ag+ released under NIR radiation endowed the NP hydrogel with prominent antibacterial properties against Escherichia coli (E. coli) and methicillin-resistant Staphylococcus aureus (MRSA), with an inhibition rate of 99.7% and 99.8%, respectively. In vivo wound healing experiments indicated that the NP hydrogel could enhance bacterial clearance, increase collagen coverage area and up-regulate VEGF expression, exhibiting high biocompatibility. Overall, this study proposed an efficient and highly biocompatible multi-modal therapeutic nanohydrogel, opening up a new way for developing broad-spectrum antibacterial wound dressings to treat bacterial wound infections. STATEMENT OF SIGNIFICANCE: Bacterial wound infection is still one of the most difficult medical problems. In this work, a stimulating NIR-responsive hydrogel encapsulating functional Ag2S QDs was prepared, which showed high photothermal conversion efficiency (57.3%) and outstanding antibacterial ability under 808 nm NIR laser, killing 99.7% and 99.8% of E. coli and MRSA in 4 min, respectively. During NIR light irradiation, the release rate of Ag+ could be regulated by the intrinsic volume transition of the hydrogel, leading to remarkable antibacterial properties in vitro and in vivo under the combined action of hyperthermia, radical oxygen species and Ag+ released. This study proposed a novel multi-modal therapeutic nanohydrogel, opening up a new way for developing broad-spectrum antibacterial wound dressings to treat bacterial wound infections.

Memristive Behaviors Dominated by Reversible Nucleation Dynamics of Phase-Change Nanoclusters.

One of the important steps for realizing artificial intelligence is identifying elementary units that are beneficial for neural network construction. A type of memristive behavior in which phase-change nanoclusters nucleate adaptively in two adjacent dielectric layers with distinct distribution patterns is demonstrated. This memristive system responds in potentiation to increased stimulation strength and fire action potential after threshold stimulation. Reversible nucleation of phase-change nanoclusters is confirmed after both in situ and ex situ examinations using high-resolution transmission electron microscopy. The dynamics at the nanoscale level dominates the actions of the two dielectric layers. The oscillation response over a long period is due to the competition between crystalline and amorphous phases in the layer near the bottom electrode. Weight mutation, that is, action potential firing, is caused by the blockage of the filament in the layer near the top electrode. The memristive system is compact and able to execute complicated functions of a complete neuron and performs an important role in neuromorphic computing.

New semen freezing method for chicken and drake using dimethylacetamide as the cryoprotectant.

The aim is to optimize the dimethylacetamide (DMA) straw freezing technology of Black silkies rooster semen through the handy patent equipment, screening the formula of freezing basic extender and optimizing the DMA addition method, and then by comparing the fertility of DMA straw frozen semen with the pellet frozen semen. After the DMA straw freezing technology is optimized, it is extended to the Youxian Partridge drake semen. The result showed that the frozen sperm motility of Lake and Ravie (LR) group is 64%, the fertility 49.57% and the hatchability 91.52%, all of which are superior to those of FEB, Beltsville Poultry Semen Extender (BPSE) and Lake (P < 0.05). The sperm motility of adding DMA stock solution is 59%, which is superior to adding DMA directly into diluted semen (P > 0.05). The fertility and hatchability of DMA straw group are 77.61% and 92.30%, respectively, and it is significantly higher than those in the pellet group (P < 0.01; P < 0.05). The fresh drake sperm motility of induction collection method is 71%, the massage collection method 61% and the frozen drake sperm motility of induction 33% while the massage 19%. The fertility of frozen drake semen group is 85.93%, while that of the fresh semen group is 88.17%. The frozen drake semen fertility of the highest batch is 93.8%. In conclusion, the world's advanced fertility of frozen semen can be obtained both in the chicken and drake through the optimized DMA straw freezing technology and the method of screening freeze-resistant individuals.

Electrochemical and thermodynamic properties of 1-phenyl-3-(phenylamino)propan-1-one with Na2WO4 on N80 steel.

The corrosion inhibition effect and adsorption behaviour of 1-phenyl-3-(phenylamino)propan-1-one (PPAPO) on N80 steel in hydrochloric acid solution have been investigated by Fourier transform infrared (FTIR), electrochemical method and scanning electron microscopy. The corrosion inhibition mechanism of PPAPO mixed with Na2WO4 was interpreted from the thermodynamic point of view. The results indicated that PPAPO mixed with Na2WO4 acted as a mixed-type inhibitor. The inhibition film formed on N80 steel surface can increase the charge transfer resistance and prevent the occurrence of corrosion reaction, thereby reducing the corrosion rate of metal surface. The inhibition efficiency was up to 96.65%; the inhibitor PPAPO with Na2WO4 showed good synergistic effect on N80 corrosion behaviour in HCl solution. The adsorption behaviour of inhibitors on N80 steel surface was in accordance with the Langmuir adsorption model and mainly belonged to chemisorption. The adsorption process of PPAPO on N80 surface was spontaneous and irreversible endothermic reaction.

Giant polarization in super-tetragonal thin films through interphase strain.

Strain engineering has emerged as a powerful tool to enhance the performance of known functional materials. Here we demonstrate a general and practical method to obtain super-tetragonality and giant polarization using interphase strain. We use this method to create an out-of-plane-to-in-plane lattice parameter ratio of 1.238 in epitaxial composite thin films of tetragonal lead titanate (PbTiO3), compared to 1.065 in bulk. These thin films with super-tetragonal structure possess a giant remanent polarization, 236.3 microcoulombs per square centimeter, which is almost twice the value of known ferroelectrics. The super-tetragonal phase is stable up to 725°C, compared to the bulk transition temperature of 490°C. The interphase-strain approach could enhance the physical properties of other functional materials.

The formation of heterointerface defects in Au/Cu films on Si substrates under direct current in a vacuum ultraviolet environment.

Au/Cu metallic films were deposited on p-Si(100) substrates with and without an Au upper layer by magnetron sputtering. The defect formation and nanoscale interfacial evolution at the Au/Cu and Cu/Si interfaces were studied by using Auger electron spectroscopy (AES) and high resolution transmission electron microscopy (HRTEM). The results showed that an increase in defects at the heterointerfaces and in the surface layer was induced by the effect of a direct current (DC) in a vacuum ultraviolet (UV) environment, which could provide more channels for the removal of atoms. The directed migration of atomic clusters in the films was caused by the effect of the DC, which also aggravated the defects' expansion and led to the formation of Au-Cu intermetallic compounds (IMCs). In addition, the voids formed at the interface between the Au/Cu films and the Si substrates were found to be mainly related to the generation of the material Au2Cu3.

Lattice distortion and orbital hybridization in NdFeO3-PbTiO3 ferroelectric thin films.

Single-phase xNdFeO3-(1 - x)PbTiO3 thin films with different dopant contents were fabricated on the Pt(111)/Ti/SiO2/Si substrate by a sol-gel route. Grain size was influenced by the dopant content effectively. A synchrotron radiation X-ray diffraction study revealed a reduced tetragonality (c/a) of the PbTiO3 lattice in the films. Distortion of the TiO6 octahedron was weakened, as investigated by Raman scattering and X-ray absorption spectra. An electronic structural study indicated that the hybridizations between O 2p and Pb 6s and Ti 3d orbitals were weakened. The decrease of lattice distortion and orbital hybridization gives rise to degradation of the ferroelectric nature in the films.

Hydrogen Impurity Defects in Rutile TiO2.

Hydrogen-related defects play crucial roles in determining physical properties of their host oxides. In this work, we report our systematic experimental and theoretical (based on density functional theory) studies of the defect states formed in hydrogenated-rutile TiO2 in gaseous H2 and atomic H. In gas-hydrogenated TiO2, the incorporated hydrogen tends to occupy the oxygen vacancy site and negatively charged. The incorporated hydrogen takes the interstitial position in atom-hydrogenated TiO2, forming a weak O-H bond with the closest oxygen ion, and becomes positive. Both states of hydrogen affect the electronic structure of TiO2 mainly through changes of Ti 3d and O 2p states instead of the direct contributions of hydrogen. The resulted electronic structures of the hydrogenated TiO2 are manifested in modifications of the electrical and optical properties that will be useful for the design of new materials capable for green energy economy.

Insight into Metalized Interfaces in Nano Devices by Surface Analytical Techniques.

Connections between metals and heterogeneous solid state materials form buried interfaces. These ubiquitous structures play an essential role in determining the performances of many nano- and microdevices. However, the information about the chemistry, structure, and properties of these real interfaces is intrinsically difficult to extract by traditional techniques. Therefore, approaches to efficiently discovering metalized interfaces are in high demand. Here, we demonstrate the transformation of nanoscale metal/oxide interface problems into surface problems through a novel metal-hydrogenation detaching method. We applied this technique to study the thickness dependence in Pb(Zr,Ti)O3 (PZT) ferroelectric thin films, a long-standing interface problem in a model metal/insulator device, and this allowed comprehensive surface analytical techniques to be adapted. A nonstoichiometric interfacial layer of 4.1 nm thick with low mass density, low permittivity, and weak ferroelectricity was quantified at the Pt/PZT interface and attributed to the preferential diffusions among the compositional elements. Targeted interface engineering by Pb rebalance led to a substantial recovery of ferroelectric properties. Our results therefore pave the way to a better understanding of metallized interface in ferroelectric and dielectric nanodevices. We hope that more useful information about metalized interfaces of other solid materials could, analogously, be accessed by surface analytical techniques.

Giant conductivity enhancement of ferrite insulators induced by atomic hydrogen.

Hydrogen behavior in oxides has triggered much interest for its scientific and technological importance in a wide range of research fields from novel ion conductors to astrochemistry. Here, we report a giant conductivity enhancement in ZnFe2O4 ferrite insulators to the metallic state by over eleven orders of magnitude induced by electrochemically generated atomic hydrogen at room temperature. The conductivity and the amount of incorporated hydrogen increased in an exponential function with time. An activation energy for the atomic hydrogen chemisorption was measured to be 8.23 kJ mol(-1). Quantitative kinetics correlations among the adsorption of atomic hydrogen, hydrogen incorporation and conductivity enhancement are established, based on which hydrogen incorporation process is clarified herein. We demonstrate that the hydrogen incorporation in oxides can be adjusted by manipulating the kinetic factors. These findings have implications for research into hydrogen behavior in oxides in environments containing hydrogen atoms and offer possibilities for utilizing and controlling the modifications of oxide materials induced by atomic hydrogen.

Ultra-low percolation threshold in ferrite-metal cofired ceramics brings both high permeability and high permittivity.

High permeability and high permittivity are hard to be achieved simultaneously, either in single-phased materials or in composite materials, such as ferrite-ferroelectric ceramic composites and ferrite-metal percolative composites. In this work, ultra-low percolation threshold is achieved in NiZnCu ferrite-Ag cofired ceramics, which endows the composite with both high permeability and high permittivity by minimizing the negative effect of nonmagnetic conductive fillers on magnetic properties. The percolation threshold is controlled by the temperature matching between ferrite densification and Ag melting. A thin and long percolative net forms between large ferrite grains under a proper cofiring process, which brings a low percolation threshold of 1.21vol%, more than one order of magnitude lower than the theoretical value of 16vol%. Near the ultra-low threshold, the composite exhibits a high permeability of 585 and a high permittivity of 78.

Electron migration behavior of Au/Cu multilayer films on Si substrates under UV radiation.

Au/Cu multilayer films were plated by the magnetron sputtering method on p-Si(100) substrates. The sample temperature was changed from room temperature to 44 °C under UV radiation in a vacuum within 120 minutes, and then remained stable with treatment time increased. Meanwhile, the surface roughness was changed from 4.2 nm to 5.9 nm and then also remained stable. But the interface width of Au/Cu still continued to increase during that steady stage. The calculation results show that the concentration gradient of Cu atoms fell to 2.24 in 360 minutes from 3.45 at the beginning. The increase of defects in the grain boundaries of the Au layer was induced by UV radiation, because the Cu element had a smaller work function relative to the Au element and it was more likely to migrate to the surface layer through the grain boundaries of the Au layer.