Antimicrobial Peptide-Inspired Design of Amino-Modified Lignin with Improved Antimicrobial Activities.

A major challenge to make use of lignin as an antimicrobial material is the weak antimicrobial activity of industrial lignin. Inspired by the antimicrobial mechanism of actions of antimicrobial peptides, alkyldiamines were employed as lysine mimics for lignin modifications. Accordingly, aminoalkyl-modified lignins with different degrees of substitution of amino groups and different hydrophobicity were synthesized. The chemical structure, properties, and antimicrobial activities of the as-prepared aminoalkyl lignins were thoroughly characterized with state-of-the-art technologies. The results indicated that aminobutyl lignin showed enhanced antimicrobial activity against S. aureus and E. coli and performed even better than copper ions. The antimicrobial mechanism of action of the as-prepared aminobutyl lignin was similar to that of polylysine, which damaged the cell membrane, leading to the leakage of intracellular molecules and death of the cell. This study provides a feasible approach to afford modified lignin with enhanced antimicrobial performance, which would facilitate the high-value valorization of lignin as biological materials.

Visible light-regulated cationic polymer coupled with photodynamic inactivation as an effective tool for pathogen and biofilm elimination.

BACKGROUND: Pathogenic microorganism pollution has been a challenging public safety issue, attracting considerable scientific interest. A more problematic aspect of this phenomenon is that planktonic bacteria exacerbate biofilm formation. There is an overwhelming demand for developing ultra-efficient, anti-drug resistance, and biocompatibility alternatives to eliminate stubborn pathogenic strains and biofilms. RESULTS: The present work aims to construct a visible light-induced anti-pathogen agents to ablate biofilms using the complementary merits of ROS and cationic polymers. The photosensitizer chlorin e6-loaded polyethyleneimine-based micelle (Ce6-TPP-PEI) was constructed by an amphiphilic dendritic polymer (TPP-PEI) and physically loaded with photosensitizer chlorin e6. Cationic polymers can promote the interaction between photosensitizer and Gram-negative bacteria, resulting in enhanced targeting of PS and lethality of photodynamic therapy, and remain active for a longer duration to prevent bacterial re-growth when the light is turned off. As expected, an eminent antibacterial effect was observed on the Gram-negative Escherichia coli, which is usually insensitive to photosensitizers. Surprisingly, the cationic polymer and photodynamic combination also exert significant inhibitory and ablative effects on fungi and biofilms. Subsequently, cell hemolysis assessments suggested its good biocompatibility. CONCLUSIONS: Given the above results, the platform developed in this work is an efficient and safe tool for public healthcare and environmental remediation.

Purification and molecular weight distribution of a key exopolysaccharide component of Bacillus megaterium TF10.

Extracellular polymeric substances (EPS) are organic metabolic compounds excreted by microorganisms. They largely impact microbial aggregate structures and functions. Extracellular polysaccharides (EP) in EPS are responsible for the formation of microbial aggregates. In this work, we successfully separated and characterized EP from EPS of the bacterium Bacillus megaterium TF10. Extraction of EP from EPS was optimized using Sevag's reagent. Chemical characteristics, functional groups, and molecular weight (MW) distribution of EP were compared with the harvested EPS and soluble microbial products (SMP). We found that the polymers of lower MW and free proteins were successfully removed by Sevag's reagent. The higher MW components of EPS were predominantly polysaccharides, while the polymers of lower MW tended to secrete to the supernatant and were described as SMP. A part of the proteins in the EP was polysaccharide-bonded. Our results can be further used in elucidating the complex flocculation mechanisms in which EP play a major role.

Enhanced osteogenic and bactericidal performance of premixed calcium phosphate cement with photocrosslinked alginate thin film.

The increasing prevalence of implant-associated infections (IAI) in orthopedics remains a public health challenge. Calcium phosphates (CaPs) are critical biomaterials in dental treatments and bone regeneration. It is highly desirable to endow CaPs with antibacterial properties. To achieve this purpose, we developed a photocrosslinked methacrylated alginate co-calcium phosphate cement (PMA-co-PCPC) with antibacterial properties, using α-tricalcium phosphate (α-TCP) powders with 16% amorphous contents as solid phase, liquid phases containing CuCl2 and SrCl2 as an inhibitor, and CaCl2 as an activator to construct PCPC. When CaCl2 started to activate the hydration reaction, Sr2+ or Cu2+ ions were exchanged with Ca2+, and α-TCP dissolution was restarted and gradually hydrated to form calcium-deficient hydroxyapatite (CDHA). PMA was added to crosslink with Cu/Sr ions and form gel-layer-wrapped hydrated CDHA. This study explored the binding mechanism of PMA and PCPC and the ion release rule of Ca2+ → Sr2+/Cu2+, optimized the construction of several antibacterial PMA-co-PCPC materials, and analyzed the physical, chemical, and biological properties. Because of the combined effect of Cu and Sr ions, the scaffold exhibited a potential antibacterial activity, promoting bone formation and vascular regeneration. This work provides a basis for designing antibacterial calcium phosphate biomaterials with controllable treatment, which is an important characteristic for preventing IAI of biomaterials.

Preparation and antibacterial property of waterborne polyurethane/Zn-Al layered double hydroxides/ZnO nanocomposites.

In this work, a novel environmental-friendly waterborne polyurethane/ZnAl-layered double hydroxides/ZnO nanoparticles composite (WPU/ZnAl-LDHs/ZnO) was synthesized via in-situ polymerization. ZnAl-LDHs and ZnAl-LDHs/ZnO were synthesized by refluxing in an oil bath. In order to disperse ZnAl-LDHs/ZnO homogeneously into WPU matrix, ZnAl-LDHs/ZnO was firstly functionalized by isophorone diisocyanate. The incorporated content of ZnAl-LDHs/ZnO in the composite has profound effect on such physical properties as mechanical strength, thermal stability and water swelling. It is demonstrated that appropriate amount of ZnAl-LDHs/ZnO with good dispersion in the WPU matrix significantly improves the physical performance of the composites. Finally, the antibacterial activity of the composite was tested against G(-) Escherichia coli and G(+) Staphylococcus aureus. The results indicate that WPU incorporated with ZnAl-LDHs/ZnO shows strong antibacterial activity upon contact.

Selecting Suitable Near-Native Lignins for Research.

There are several methods to isolate near-native lignins, including milled-wood lignin, enzymatic lignin, cellulolytic enzyme lignin, and enzymatic mild-acidolysis lignin. Which one is the most representative of the native lignin? Herein, near-native lignins were isolated from different plant groups and structurally analyzed to determine how well these lignins represented their native lignin counterparts. Analytical methods were applied to understand the molecular weight, monomer composition, and distribution of interunit linkages in the structure of the lignins. The results indicated that either enzymatic lignin or cellulolytic enzyme lignin may be used to represent native lignin in softwoods and hardwoods. None of the lignins, however, appeared to represent native lignins in grasses (monocot plants) because of substantial syringyl/guaiacyl differences. Complicating the understanding of grass lignin structure, large amounts of hydroxycinnamates acylate their polysaccharides and, when released, are often conflated with actual lignin monomers.

Microbiologically Influenced Corrosion of Q235 Carbon Steel by Ectothiorhodospira sp.

The biological sulfur cycle is closely related to iron corrosion in the natural environment. The effect of the sulfur-oxidising bacterium Ectothiorhodospira sp., named PHS-Q, on the metal corrosion behaviour rarely has been investigated. In this study, the corrosion mechanism of Q235 carbon steel in a PHS-Q-inoculated medium is discussed via the characterization of the morphology and the composition of the corrosion products, the measurement of local corrosion and the investigation of its electrochemical behaviour. The results suggested that, initially, PHS-Q assimilates sulfate to produce H2S directly or indirectly in the medium without sulfide. H2S reacts with Fe2+ to form an inert film on the coupon surface. Then, in localised areas, bacteria adhere to the reaction product and use the oxidation of FeS as a hydrogen donor. This process leads to a large cathode and a small anode, which incurs pitting corrosion. Consequently, the effect of PHS-Q on carbon steel corrosion behaviour is crucial in an anaerobic environment.

Surface-modified polylactic acid nanospheres with chitosan for antibacterial activity of 1, 2-benzisothiazolin-3-one.

The primary purpose of this study was to develop an innovative chitosan (CS) modified polylactic acid (PLA) nanospheres for enhancing the bioavailability of 1, 2-benzisothiazolin-3-one (BIT). The cellular uptake efficiency was corresponded positively to the quantity of CS coated on BIT-PLA nanospheres against E. coli and S. aureus. The membrane potentials of E.coli and S. aureus treated with BIT-PLA, BIT-PLA-0.1%CS and BIT-PLA-0.5%CS were reduced with the extension of incubation time and the ratio of coated CS. The enhancement of CS modified on BIT-PLA nanospheres was reduced antioxidase activities and generated excessive reactive oxygen species. The lowest EC50 value of the modified BIT-PLA-0.5%CS suggested that its toxicity index was around 2.95-fold and 2.11-fold that of non-modified BIT-PLA against E. coli and S. aureus, respectively. These results revealed that the CS modified BIT-PLA nanospheres had a bright prospect in antibacterial formulation delivery system and improving the bioavailability.

Enhanced photodynamic inactivation for Gram-negative bacteria by branched polyethylenimine-containing nanoparticles under visible light irradiation.

Antibiotic pollution has been a serious global public health concern in recent years, photodynamic inactivation is one of the most promising and innovative methods for antibacterial applications that avoids antibiotic abuse and minimizes risks of antibiotic resistance. However, limited by the weak interaction between the photosensitizers and Gram-negative bacteria, the effect of photodynamic inactivation cannot be fully exerted. Herein, photosensitizer chlorin e6-loaded polyethyleneimine-based micelle was constructed. The synergy of electrostatic and hydrophobic interactions between the nanoparticles and the bacterial surface promoted the anchoring of nanoparticles onto the bacteria, resulting in enhanced photoinactivation activities on Gram-negative bacteria. As expected, an eminent antibacterial effect was also observed on the Gram-positive bacteria Staphylococcus aureus. The cellular uptake results showed that photosensitizer was firmly anchored to the bacterial cell surface of Escherichia coli or Staphylococcus aureus by the introduction of branched polyethylenimine-containing nanoparticles. The light-triggered generation of reactive oxygen species, mainly singlet oxygen, from the membrane-bound nanoparticles caused irreversible damage to the bacterial outer membrane, achieving enhanced bactericidal efficiency than free photosensitizer. The study would provide an efficient and promising antimicrobial alternative to prevent overuse of antibiotics and have enormous potential for human healthcare and the environment remediation.

Cetylpyridinium bromide/montmorillonite-graphene oxide composite with good antibacterial activity.

In this study, a cetylpyridinium bromide (CPB)/montmorillonite-graphene oxide (GM) composite (GM-CPB) was prepared by loading CPB in a carrier of GM. The chemical structure, elemental composition, morphology, thermogravimetric analysis, antibacterial activity, sustained release property and cytotoxicity were analyzed. The loading rate of CPB in a GM carrier was higher than that of the graphene oxide (GO) carrier under the same loading condition. The antibacterial activity and sustained release performance of GM-CPB were also better than that of GO-CPB; furthermore, GM-CPB showed lower cytotoxicity than CPB.

Combined delivery of bone morphogenetic protein-2 and insulin-like growth factor-1 from nano-poly (γ-glutamic acid)/ß-tricalcium phosphate-based calcium phosphate cement and its effect on bone regeneration in vitro.

In this study, nano-doped calcium phosphate cement delivery systems (poly (γ-glutamic acid)/ß-tricalcium phosphate/calcium phosphate ceramics and nano (γ-glutamic acid)/ß-tricalcium phosphate/calcium phosphate ceramic) were fabricated, and low doses (10 µg/g) of two growth factors, insulin-like growth factor-1 and bone morphogenetic protein-2, were encapsulated then sequentially released. We characterized the delivery systems using Fourier transform infrared spectroscopy and X-ray diffraction and measured washout resistance and compressive strength, and thus optimized the most appropriate proportioning of delivery systems for the two growth factors. One of the growth factors was absorbed by the nano-poly (γ-glutamic acid)/ß-tricalcium phosphate, which was then mixed into the calcium phosphate ceramic solid phase to create a new solid phase calcium phosphate ceramic. Nano-poly (γ-glutamic acid)/ß-tricalcium phosphate/calcium phosphate ceramic carriers were then prepared by blending the new calcium phosphate ceramic solid phase powder with a solution of the remaining growth factor. The effects of different release patterns (studying sequential behavior) of insulin-like growth factor-1 and bone morphogenetic protein-2 on osteogenic proliferation and differentiation of the MC3t3-E1 mouse osteoblast cell were investigated. This combinational delivery system provided a controlled release of the two growth factors, in which nano-doping significantly affected their release kinetics. The incorporation of dual growth factors could potentially stimulate bone healing and promoting bone ingrowth processes at a low dose.

Poly (γ-glutamic acid)/beta-TCP nanocomposites via in situ copolymerization: Preparation and characterization.

A series biodegradable poly (γ-glutamic acid)/beta-tricalcium phosphate (γ-PGA/TCP) nanocomposites were prepared which were composed of poly-γ-glutamic acid polymerized in situ with ß-tricalcium phosphate and physiochemically characterized as bone graft substitutes. The particle size via dynamic light scattering, the direct morphological characterization via transmission electron microscopy and field emission scanning electron microscope, which showed that γ-PGA and ß-TCP were combined compactly at 80℃, and the γ-PGA/TCP nanocomposites had homogenous and nano-sized grains with narrow particle size distributions. The water uptake and retention abilities, in vitro degradation properties, cytotoxicity in the simulated medium, and protein release of these novel γ-PGA/TCP composites were investigated. Cell proliferation in composites was nearly twice than ß-TCP when checked in vitro using MC3T3 cell line. We also envision the potential use of γ-PGA/TCP systems in bone growth factor or orthopedic drug delivery applications in future bone tissue engineering applications. These observations suggest that the γ-PGA/TCP are novel nanocomposites with great potential for application in the field of bone tissue engineering.