Chemically Modulating Ceria-Based Artificial Haloperoxidase for Enhanced Antibacterial Activity and Biofilm Inhibition.

Ceria (CeO2) nanoparticles with haloperoxidase (HPO)-like activity have gained attention as a biologically benign antifoulant. 3,4-Dihydroxy-l-phenylalanine (DOPA), a main composition in mussel foot proteins, plays a crucial role in the biofouling process. However, the impact on the HPO-like activity and antifouling performance of CeO2 nanoparticles when DOPA molecules adsorb on them remains unexplored. This interesting question warrants investigation, particularly considering that it may occur in an actual marine environment. Herein, the interaction between DOPA and CeO2 is explored. Despite the higher Ce3+ fractions and the lower band gap energies due to the electron transfer from DOPA to the CeO2 surface, DOPA still had a slightly negative effect on the HPO-like activity of CeO2 since they decreased the exposed Ce3+ sites. The DOPA-CeO2 nanocomposites with HPO-like activities could kill bacteria and trigger quorum-sensing signaling quenching, achieving a biofilm inhibition performance. Amazingly, 0.1% DOPA-CeO2 nanocomposite exhibited higher antibacterial activity and better biofilm suppression activities due to its HPO-like activity and positive zeta potential. The remarkable results demonstrated that DOPA, as a participant in the biofouling process, could enhance the antibacterial activity and antifouling performance of CeO2 nanoparticles at an appropriate concentration.

Facet-dependent haloperoxidase-like activities of CeO2 nanoparticles contribute to their excellent biofilm formation suppression abilities.

Biofilms adhering to different surfaces have significant negative impacts in various fields. Cerium oxide nanoparticles can serve as mimics of haloperoxidase for biological biofilm inhibition applications. The regulation of the exposed facet of CeO2 nanoparticles influences their efficiency in various catalytic processes. However, there is still a lack of systematic studies on the facet-dependent haloperoxidase-like activity of CeO2. In the present study, the facet-dependent haloperoxidase activities and antibiofilm performance of CeO2 nanoparticles were elucidated through experiment analysis and density function theory calculation. The as-prepared CeO2 nanoparticles inhibited bacterial survival and catalyzed the oxidative bromination of quorum sensing signaling molecules, achieving biofilm inhibition performance. The antibacterial and biofilm formation suppression abilities were consistent with their haloperoxidase activities. The {111}- and {110}-facet CeO2 nanopolyhedra, as well as the {110}- and {100}-facet CeO2 nanorods, which had higher haloperoxidase activity showed better antibiofilm performance than the {100}-facet CeO2 cubes. The present findings provide a comprehensive understanding of the facet-dependent haloperoxidase-like activity of CeO2. Furthermore, engineering CeO2 morphologies with different crystal facets may represent a novel method for significantly adjusting their haloperoxidase-like activity.

RETRACTED: Liu et al. The Effect of Intrinsic Mechanical Properties on Reducing the Friction-Induced Ripples of Hard-Filler-Modified HDPE. Polymers 2023, 15, 268.

The Polymers Editorial Office retracts the article "The Effect of Intrinsic Mechanical Properties on Reducing the Friction-Induced Ripples of Hard-Filler-Modified HDPE" [...].

Antifouling applications and fabrications of biomimetic micro-structured surfaces: A review.

BACKGROUND: Since the inception of the term "Biomimetics" in 1991, the concept of utilizing natural solutions or deriving inspiration from nature to address contemporary engineering challenges has gained significant attention within the scientific community. Organisms, in order to thrive in harsh environments, have evolved a wide range of micro/nanostructured surfaces, which serve as a rich source of inspiration for the development of artificial micro/nano-structured surfaces. These natural adaptations provide valuable insights and novel pathways for fabricating such surfaces. AIM: To conclude recent advances in micro/nano-structured surfaces from four aspects: biomimetic micro-structured surfaces of plants and animals, properties and applications of biomimetic surfaces, methods of preparations, and their limitation. KEY SCIENTIFIC CONCEPTS: Artificial micro/nano-structured surfaces inspired by animals and plants are classified and demonstrated according to their living environment. The performances, principles and preparation techniques of natural superhydrophobic surfaces, slippery liquid-infused porous surfaces (SLIPS), anisotropic surfaces, etc. are described in detail. Moreover, the pros and cons of each preparation measures are compared and the challenges developing large-scale, cost-effective surface microstructure preparation processes are pointed out. In the end, the development trends of artificial micro/nano-structured surface are forecasted.

Novel Wood-Based Functional Material with Vibration and Noise Reduction.

As a kind of typical green material, natural materials tend to exhibit excellent performance in the engineering field because of their structure and special functions. The homogeneous vessels of red willow (RW) are potentially unique structures to store lubricants or reinforcing agents to present special functions for engineering applications. A series of novel red willow wood-based composites, which were infused with nano-MoS2 and then reinforced by the epoxy, were developed. Their self-lubricating, mechanical vibration and noise reduction performances were investigated, and the friction, vibration, and noise reduction mechanisms were disclosed. The infusion MoS2 treatment was very beneficial for improving the tribological properties of MoS2-curing epoxy/red willow (MCW), and the coefficient of friction (COF) was reduced by 65.8% under water-lubricated friction after infusing 24 times. Meanwhile, the mechanical performances of MCW were obviously enhanced through the curing treatment of the epoxy. The synergistic effects of the infusion and curing treatments significantly decreased the wear phenomena on the friction surfaces of MCW and weakened the COF and its fluctuation amplitudes, which resulted in the presented excellent vibration and noise reduction performance. The knowledge gained herein could not only develop a novel wood-based composite with low COF and good vibration reduction properties in the engineering field but also provide a new methodology for the design of artificial porous materials with stable and smooth friction processes.

Enhanced antifouling properties of marine antimicrobial peptides by PEGylation.

Covalent immobilisation of antimicrobial peptides (AMPs) on underwater surfaces to combat marine biofouling is of great interest as it is an efficient, broad-spectrum and environmentally friendly strategy. Similar to post-translational modifications of natural proteins, artificial modifications of antimicrobial peptides can introduce important impacts on their properties and functions. The present work revealed the enhanced effect of PEGylation on the antifouling properties of marine antimicrobial peptides (LWFYTMWH) through grafting the modified peptides on aluminium surfaces. PEG was coupled to the peptide by solid-phase peptide synthesis, and the PEGylated peptides were bioconjugated to the aluminium surfaces which was pre-treated by aryldiazonium salts to introduce carboxyl groups. The carboxy group has been activated through the reaction with 1-(3-dimethylaminopropyl)-3-ethylcarbodiimide hydrochloride and N-hydroxysuccinimide. The successful modification was confirmed via FT-IR and XPS. Interestingly, the PEGylated peptides modified surfaces could kill 90.0% Escherichia coli (Gram-negative) and 76.1% Bacillus sp. (Gram-positive), and showed better antifouling performance than the original peptides modified surfaces. Furthermore, molecular dynamics simulations showed PEGylation could enhance the ability of peptides to destroy membrane. The PEGylated peptides inserted into the membrane and induced the change in local curvature of membrane, leading to the rupture of membrane. The presence of PEG changed the antimicrobial peptides into more flexible conformations and the high hydrophilicity of PEG hindered the settlement of bacteria. These might be the two main working mechanisms for the increased antifouling efficiency of PEGylated peptides modified surface. This study provided a feasible modification strategy of antimicrobial peptides to enhance their antifouling properties.

The Effect of Intrinsic Mechanical Properties on Reducing the Friction-Induced Ripples of Hard-Filler-Modified HDPE.

Ripple deformations induced by friction on polymeric materials have negative effects on the entire stability of operating machineries. These deformations are formed as a response to contacting mechanics, caused by the intrinsic mechanical properties. High-density polyethylene (HDPE) with varying silicon nitride (Si3N4) contents is used to investigate different ripple deformation responses by conducting single-asperity scratch tests. The relationship between the intrinsic mechanical properties and the ripple deformations caused by filler modifications is analyzed in this paper. The results show the coupling of the inherent mechanical properties, and the stick-slip motion of HDPE creates ripple deformations during scratching. The addition of the Si3N4 filler changes the frictional response; the filler weakens the ripples and almost smoothens the scratch, particularly at 4 wt.%, but the continued increase in the Si3N4 content produces noticeable ripples and fluctuations. These notable differences can be attributed to the yield and post-yield responses; the high yield stress and strain-hardening at 4 wt.% provide good friction resistance and stress distribution, thus a smooth scratch is observed. In contrast, increasing the filler content weakens both the yield and post-yield responses, leading to deformation. The results herein reveal the mechanism behind the initial ripple deformation, thus providing fundamental insights into universally derived friction-induced ripples.

Integration of Antifouling and Underwater Sound Absorption Properties into PDMS/MWCNT/SiO2 Coatings.

Any surface immersed in sea water will suffer from marine fouling, including underwater sound absorption coatings. Traditional underwater sound absorption coatings rely heavily on the use of toxic, biocide-containing paints to combat biofouling. In this paper, an environmentally-friendly nanocomposite with integrated antifouling and underwater sound absorption properties was fabricated by adopting MWCNTs-COOH and SiO2 into PDMS at different ratios. SEM, FTIR and XPS results demonstrated MWCNTs were mixed into PDMS, and the changes in elements were also analyzed. SiO2 nanoparticles in PDMS decreased the tensile properties of the coating, while erosion resistance was enhanced. Antibacterial properties of the coatings containing MWCNTs-COOH and SiO2 at a ratio of 1:1, 1:3, and 1:5 reached 62.02%, 72.36%, and 74.69%, respectively. In the frequency range of 1500-5000 Hz, the average sound absorption coefficient of PDMS increased from 0.5 to greater than 0.8 after adding MWCNTs-COOH and SiO2, which illustrated that the addition of nanoparticles enhanced the underwater sound absorption performance of the coating. Incorporating MWCNTs-COOH and SiO2 nanoparticles into the PDMS matrix to improve its sound absorption and surface antifouling properties provides a promising idea for marine applications.

Tribological behavior of cellulose nanocrystal as an eco-friendly additive in lithium-based greases.

The development of eco-friendly lubricant additives is of great significance for environmental protection. In this study, cellulose nanocrystal (CNC) was prepared and added into four lithium-based greases with different consistencies and apparent viscosities. The results suggest that the concentration of doped CNC should be limited to a certain value (5 wt% to 10 wt% depending on the grease type) to avoid excessive variation on the basic physical properties of greases. In the pristine grease with low consistency (NLGI grade 1) the incorporated CNC could be effectively transported through the fibrous network and deposited on the sliding surface. Through the surface mending and protection by CNC additive, together with the strong hydrodynamic effect of the high viscous base oil (220 cSt at 40 °C), the biggest reduction of friction and wear was achieved by 16% and 29% respectively. This study reveals the lubrication mechanism and application strategy of CNC in greases.

The Reduction in the Deformation of HDPE Composites Using Self-Lubricating Fillers in an Aqueous Environment.

Reducing the deformation of polymer matrix materials can decrease the fluctuation of coefficient of friction (COF), and friction-induced vibration and its amplitudes. HDPE composites with T-ZnOw as a fixed strengthening filler were modified with the addition of Si3N4 particles at different concentrations. The COFs, wear rates, micro-morphologies, and friction-induced vibrations were obtained by conducting sliding tests against carbon steel balls in an aqueous environment at a low velocity and high load. The mechanism of the reduction in frictional fluctuation due to the addition of Si3N4 particles was revealed through the frictional responses. The results demonstrated that 4 wt% addition of Si3N4 in HDPE can enhance the strain-stress property and improve the lubrication by forming a lubricating film. Therefore, the surface deformation and the fluctuations of COFs and its vibrations were reduced. The aggregation phenomenon and reduced strain-stress response at a high concentration of Si3N4 disrupted the positive fluctuating reduction, and resulted in a rough surface with severe tearing and cracking deformations. Additionally, it led to fluctuating wear behaviors with high COF and vibrations. The results obtained in this study can elucidate the effects of adding Si3N4 particles to enhance lubrication in polymer composites. Additionally, the results provide a new research method for designing and manufacturing polymer-based composites with low friction-induced fluctuations.

Antibacterial properties of Magainin II peptide onto 304 stainless steel surfaces: A comparison study of two dopamine modification methods.

Marine biofouling is perplexing the development of marine industry, and the traditional antifouling methods are restricted by the requirements of marine environmental friendliness. Marine bacteria attachment is the initial stage of marine fouling and it can be effectively reduced by reducing bacterial attachment. In this study, two modification methods were reported to synthesize antibacterial surfaces based on the different order of Magainin Ⅱ (MAG Ⅱ) modification. The preparation of SS-DA-M was generated by modifying the 304 stainless steel (304 SS) surface with dopamine firstly and then grafting the MAG Ⅱ onto the dopamine modified surface; SS-M-DA was obtained by modifying 304 SS surface using MAG Ⅱ derivative which synthesized by MAG Ⅱ and dopamine under weak acid condition. XPS, contact angle, film thickness and surface topography analysis showed that both methods grafted MAG Ⅱ onto the 304 SS surface successfully, changing the morphology and wettability of the substrates. Antibacterial results demonstrated that the two modified surfaces possessed strong resistance against V. natriegens, and the antibacterial efficiency of SS-DA-M and SS-M-DA reached 98.07 % and 99.79 %, respectively. Robustness results illustrated that the modified surface could keep strong antibacterial capacity in seawater for a long time. The phy-chemical properties and antibacterial properties of SS-M-DA surface were superior to SS-DA-M surface because more MAG Ⅱ were grafted onto 304 SS surface and the distribution was more uniform than the SS-DA-M surface. The investigation may offer a new and promising strategy to tackle surface fouling of hull, aquaculture cage and other marine facilities.

Synthesis of magnetic nanoparticles with an IDA or TED modified surface for purification and immobilization of poly-histidine tagged proteins.

Magnetic nanoparticles (MNPs) chelating with metal ions can specifically interact with poly-histidine peptides and facilitate immobilization and purification of proteins with poly-histidine tags. Fabrication of MNPs is generally complicated and time consuming. In this paper, we report the preparation of Ni(ii) ion chelated MNPs (Ni-MNPs) in two stages for protein immobilization and purification. In the first stage, organic ligands including pentadentate tris (carboxymethyl) ethylenediamine (TED) and tridentate iminodiacetic acid (IDA) and inorganic Fe3O4-SiO2 MNPs were synthesized separately. In the next stage, ligands were grafted to the surface of MNPs and MNPs with a TED or IDA modified surface were acquired, followed by chelating with Ni(ii) ions. The Ni(ii) ion chelated forms of MNPs (Ni-MNPs) were characterized including morphology, surface charge, structure, size distribution and magnetic response. Taking a his-tagged glycoside hydrolase DspB (Dispersin B) as the protein representative, specific interactions were confirmed between DspB and Ni-MNPs. Purification of his-tagged DspB was achieved with Ni-MNPs that exhibited better performance in terms of purity and activity of DspB than commercial Ni-NTA. Ni-MNPs as enzyme carriers for DspB also exhibited good compatibility and reasonable reusability as well as improved performance in various conditions.

Role of trapped air and lubricant in the interactions between fouling and SiO2 nanoparticle surfaces.

Both biomimetic superhydrophobic surfaces and biomimetic slippery liquid-infused porous surfaces (SLIPSs) have been developed as potential alternatives for solving the problem of biofouling. Herein, a facile method was used to construct superhydrophobic surfaces and liquid infused porous surfaces on stainless steels for antifouling applications. The nano-structures were formed by electrostatic attraction between polycations and negatively charged SiO2 nanoparticles, providing a structural basis for superhydrophobic surfaces and liquid infused surfaces. Biofouling testing suggested excellent antifouling performances of the liquid infused porous surfaces by decreasing the adhesion of Chlorella pyrenoidosa by 93% and of Phaeodactylum tricornutum by 71%. The thermodynamic interpretation further indicated that the air layer captured by the superhydrophobic surfaces and the lubricant layer entrapped by the liquid infused porous surfaces played the dominant role in their antifouling performances. The inspiring results might show great potential for liquid infused porous surfaces in antifouling applications.

Friction reduction and viscosity modification of cellulose nanocrystals as biolubricant additives in polyalphaolefin oil.

With the increasing requirement of environmental protection, the development of lubricating materials with non-toxicity and good biodegradability becomes more and more significant. As the novel green nanomaterial derived from natural cellulose, cellulose nanocrystals (CNCs) in the present work were prepared from native cotton and added into polyalphaolefin (PAO) base oil as the lubricant additive. To improve the compatibility of CNCs with PAO, the surface of CNCs were grafted by stearoyl chains, which entangled with polyolefin chains and led to a good dispersibility and stability of the colloidal solution. This hybrid oil with the elevated viscosity improved the formation of lubricant film in the boundary lubrication regime. Combining with the mending effect of CNC particles on the surface roughness and scars, both the friction and the wear were dramatically reduced. Specifically, the introduction of 2 wt% modified nanocrystals (mCNC) in PAO base oil reduced the coefficient of friction (COF) by 30%. The results of this study suggest that cellulose nanocrystal is a promising ecofriendly and effective lubricant additive.

Magnetic immobilization of a quorum sensing signal hydrolase, AiiA.

Magnetic immobilization of quorum sensing (QS) signal hydrolases provides a convenient solution for quenching QS process that is essential for bacterial biofilm formation and antimicrobial resistance. In the present study, a QS signal hydrolase, AiiA, was fused with a magnetic protein, MagR, and expressed in Escherichia coli. Magnetic immobilization of AiiA was achieved on Fe3 O4 -SiO2 iron beads and was confirmed via SDS-PAGE, zeta potential measurement, FTIR spectrometry, and SEM analysis. The magnetic immobilized AiiA exhibited activity in degrading the quorum sensing signal, C6-HSL. This study opens a new avenue to actively immobilize enzymes via magnetic interaction and quench quorum sensing.

Rippled Polymer Surface Generated by Stick-Slip Friction.

Textured surfaces with varied functionalities are generally fabricated by etching, cutting, or printing. In this study, different from the usual generation of grooves along the sliding direction in friction, regular parallel ripples that are perpendicular to the sliding direction were generated on a polymer surface by the stick-slip friction of polymer/metal friction pairs lubricated with water. Ripple height was proportional to the peak friction force in the sticking process. Ripple wavelength decreased as the sliding velocity increased. The generation of ripples was ascribed to the adhesion and plastic deformation during stick-slip motion. The achieved rippled surface effectively improved the lubrication property of the two surfaces. These findings demonstrate a new method of in situ manufacturing ripples on a soft material surface through a controlled traditional sliding friction and also provide a new insight into the stick-slip friction behavior of materials.

A Facile Method to Prepare a Hydrophilic/Hydrophobic Metal Surface by Peptide.

A facile method to prepare a hydrophilic/hydrophobic metal surface by metal-binding peptide was proposed in this article. Metal-binding peptide sequenced NLNPNTASAMHV was taken as the target peptide to interact with stainless steel. The surface morphology, roughness and Fourier-Transform Infrared spectroscopy (FTIR) showed that some changes occurred on the modified stainless steel surface. Not only were the surfaces coarser but also some organic groups appeared on the modified sample surfaces. By comparing the CAs of all the samples, the most suitable concentration of peptide and treating time were determined. A new and facile way to endow some metals surfaces with hydrophobicity or hydrophilicity has been developed, which is useful especially for antibiofouling.

Investigation of the antibiofilm capacity of peptide-modified stainless steel.

Biofilm formation on surfaces is an important research topic in ship tribology and medical implants. In this study, dopamine and two types of synthetic peptides were designed and attached to 304 stainless steel surfaces, aiming to inhibit the formation of biofilms. A combinatory surface modification procedure was applied in which dopamine was used as a coupling agent, allowing a strong binding ability with the two peptides. X-ray photoelectron spectroscopy (XPS), elemental analysis, contact angle measurement and surface roughness test were used to evaluate the efficiency of the peptide modification. An antibiofilm assay against Staphylococcus aureus was conducted to validate the antibiofilm capacity of the peptide-modified stainless steel samples. XPS analysis confirmed that the optimal dopamine concentration was 40 µg ml-1 in the coupling reaction. Element analysis showed that dopamine and the peptides had bound to the steel surfaces. The robustness assay of the modified surface demonstrated that most peptide molecules had bound on the surface of the stainless steel firmly. The contact angle of the modified surfaces was significantly changed. Modified steel samples exhibited improved antibiofilm properties in comparison to untreated and dopamine-only counterpart, with the peptide 1 modification displaying the best antibiofilm effect. The modified surfaces showed antibacterial capacity. The antibiofilm capacity of the modified surfaces was also surface topography sensitive. The steel sample surfaces polished with 600# sandpaper exhibited stronger antibiofilm capacity than those polished with other types of sandpapers after peptide modification. These findings present valuable information for future antifouling material research.

Coupling Plant-Derived Cyclotides to Metal Surfaces: An Antibacterial and Antibiofilm Study.

Modification of metal surfaces with antimicrobial peptides is a promising approach to reduce bacterial adhesion. Here, cyclic peptides or cycloids, possessing remarkable stability and antimicrobial activities, were extracted and purified from Viola philippica Cav., and identified using mass spectrometry. Cyclotides were subsequently utilized to modify stainless steel surfaces via polydopamine-mediated coupling. The resulting cyclotide-modified surfaces were characterized by Fourier transform infrared (FTIR) spectroscopy and contact angle analysis. The antibacterial capacity of these cyclotides against Staphylococcus aureus was assessed by Alamar blue assay. The antibiofilm capacity of the modified surfaces was assessed by crystal violet assay, and scanning electron microscopy (SEM). A composite of Kalata b1, Varv A, Viba 15 and Viba 17 (P1); Varv E (P2); and Viphi G (P3) were isolated and identified. FTIR analysis of the modified surfaces demonstrated that cyclotides bound to the surfaces and induced reduction of contact angles. Antimicrobial effects showed an order P3 > P1 and P2, with P3-treated surfaces demonstrating the strongest antibiofilm capacity. SEM confirmed reduced biofilm formation for P3-treated surfaces. This study provides novel evidence for cyclotides as a new class for development of antibacterial and antibiofilm agents.

Coupling mechanism between wear and oxidation processes of 304 stainless steel in hydrogen peroxide environments.

Stainless steel is widely used in strongly oxidizing hydrogen peroxide (H2O2) environments. It is crucial to study its wear behaviour and failure mode. The tribological properties and oxidation of 304 stainless steel were investigated using a MMW-1 tribo-tester with a three-electrode setup in H2O2 solutions with different concentrations. Corrosion current densities (CCDs), coefficients of frictions (COFs), wear mass losses, wear surface topographies, and metal oxide films were analysed and compared. The results show that the wear process and oxidation process interacted significantly with each other. Increasing the concentration of H2O2 or the oxidation time was useful to form a layer of integrated, homogeneous, compact and thick metal oxide film. The dense metal oxide films with higher mechanical strengths improved the wear process and also reduced the oxidation reaction. The wear process removed the metal oxide films to increase the oxidation reaction. Theoretical data is provided for the rational design and application of friction pairs in oxidation corrosion conditions.