Biological risks of bioaerosols emitted from wastewater treatment processes have attracted wide attention in the recent years. However, the culture-based analysis method has been mostly adopted for detecting the bacte...Biological risks of bioaerosols emitted from wastewater treatment processes have attracted wide attention in the recent years. However, the culture-based analysis method has been mostly adopted for detecting the bacterial community in bioaerosols, which may result in the underestimation of total microorganism concentration as not all microorganisms are cultivable. In this study, oligonucleotide fingerprinting of 16S rRNA genes was applied to reveal the composition and structure of the bacterial community in bioaerosols from an Orbal oxidation ditch in a Beijing wastewater treatment plant (WWTP). Bioaerosols were collected at different distances from the aerosol source, rotating brushes, and the sampling height was 1.5 m which is the common respiratory height of a human being. The bacterial communities of bioaerosols were diverse, and the lowest bacterial diversity was found at the sampling site just after the rotating brush rotating brush. A large proportion of bacteria in bioaerosols were affiliated with Proteobacteria and Bacteroidetes. Numerous bacteria present in the bioaerosols also emerged in water, indicating that the bacterial community in the bioaerosols was related to that of the aerosols' sources. The forced aeration of rotating brushes brought about observably distinct bacterial communities between sampling sites situated before and after the rotating brush. Isolation sources of closest relatives in bioaerosols clone libraries were associated with the aqueous environment in the WWTP. Common potential pathogens in bioaerosols as well as those not reported in previous research were also analyzed in this study. Measures should be adopted to reduce the emission of bioaerosols and prevent their exposure to workers.展开更多
A theoretical investigation on the pH-induced switching of mixed polyelectrolyte brushes was performed by using a molecular theory. The results indicate that the switching properties of mixed polyelectrolyte brushes a...A theoretical investigation on the pH-induced switching of mixed polyelectrolyte brushes was performed by using a molecular theory. The results indicate that the switching properties of mixed polyelectrolyte brushes are dependent on the pH values. At low pH, negatively charged chains adopt a compact conformation on the bottom of the brush while positively charged chains are highly stretched away from the surface. At high pH values, the inverse transformation takes place. The role of pH determining the polymer chains conformation and charge behavior of mixed polyelectrolyte brushes was analyzed. It is found that there exists a mechanism for reducing strong electrostatic repulsions: stretching of the chains. The H+ and OH- units play a more important role as counterions of the charged polymers do. The collapse of the polyelectrolyte chains for different pH values could be attributed to the screening of the electrostatic interactions and the counterion-mediated attractive interaction along the chains.展开更多
Spherical polyelectrolyte brushes (SPBs) consisting of polystyrene (PS) core and poly(2-aminoethyl methacrylate hydrochloride) (PAEMH) shell were prepared by photo-emulsion polymerization. Au nanoparticles (A...Spherical polyelectrolyte brushes (SPBs) consisting of polystyrene (PS) core and poly(2-aminoethyl methacrylate hydrochloride) (PAEMH) shell were prepared by photo-emulsion polymerization. Au nanoparticles (Au-NPs) with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.展开更多
Nano-sized spherical polymer brushes (SPBs) consisting of both a polystyrene (PS) core and a brush shell of poly(acrylic acid) (PAA), poly(N-acrylcysteamine) (PSH), or poly(N-acrylcysteamine-co-acrylic a...Nano-sized spherical polymer brushes (SPBs) consisting of both a polystyrene (PS) core and a brush shell of poly(acrylic acid) (PAA), poly(N-acrylcysteamine) (PSH), or poly(N-acrylcysteamine-co-acrylic acid) (P(SH-co-AA)), were prepared by photo-emulsion polymerization. The core-shell structure was observed by dynamic light scattering and transmission electron microscopy. Due to the strengthened Donnan effect, the PAA brush can adsorb heavy metal ions. Effects of the contact time, thickness of PAA brush and pH value on the adsorption results were investigated. Due to the coordination between the mercapto groups and heavy metal ions as well as the electrostatic interactions, SPBs with mercapto groups are capable to remove heavy metal ions selectively from aqueous solutions. The order of adsorption capacity of the heavy metal ions by SPBs with mercapto groups is: Hg2+ ≈ Au3+ 〉 Pb2+ 〉 CH2+ 〉 Ni2+. The adsorbed heavy metal ions can be eluted from SPB by aqueous HCI solution, and the SPBs can be recovered. After three regenerations the recovered SPBs still maintain their adsorption capacity.展开更多
Polymer electrolytes a re essential for next-gene ration lithium batteries because of their excellent safety record.However,low ionic conductivity is the main obstacle restricting their commercial application.Composit...Polymer electrolytes a re essential for next-gene ration lithium batteries because of their excellent safety record.However,low ionic conductivity is the main obstacle restricting their commercial application.Composites with nanoparticles are a promising route to overcome this obstacle.In this work,lithium polystyrene sulfonate brushes(LiPSS)is anchored to silicon dioxide nanoparticles with chemical bonding using atom transfer radial polymerization(SI-ATRP).The composite polymer electrolytes are made by mixing vinylene carbonate and nanoparticles via a facile in situ polymerization process.The ionic conductivity of composite polymer electrolytes is improved to 7.2×10^-4 S/cm at room temperature,which is attributed to the low degree of crystallinity of polymer electrolyte and the fast ion transport on the surfaces of polymer brush layers that act as a conductive network.The composite polymer electrolytes show a wide electrochemical window of approximately 4.5 V vs.Li^+/Li and excellent cycling performance retention of approximately 95%after 100 cycles at ambient temperature.The results also prove that surface groups of ceramic na noparticles are an important way to increase the electrochemical properties of composite polymer electrolytes.展开更多
Hierarchical polymer brushes have been considered as an effective and promising method for preventing implant-associated infections via multiple antibacterial mechanisms.Herein,a bacterial phosphatase re-sponsive surf...Hierarchical polymer brushes have been considered as an effective and promising method for preventing implant-associated infections via multiple antibacterial mechanisms.Herein,a bacterial phosphatase re-sponsive surface with hierarchical zwitterionic structures was developed for timely dealing with the poly-meric implant-associated bacterial infection.The hierarchical polymeric architecture was subtly realized on model polypropylene(PP)substrate by sequential photo living grafting of poly(2-(dimethylamino)ethyl methacrylate(PDMAEMA)bottom layer and zwitterionic poly(sulfobetaine methacrylate)(PSBMA)upper layer,followed by the conversion of the PDMAEMA into the zwitterionic structure via succes-sive quaternization and phosphorylation reactions.Owing to shielding the bottom polycations,the hi-erarchical zwitterionic polymer brushes guaranteed the surface with the optimal biocompatibility under the normal physiological environment.Once bacteria are invaded,the surface bactericidal activity of the bottom layer can be rapidly and automatically activated owing to the transition triggered by bacterial phosphatase from zwitterion to polycation.Additionally,ameliorated by the upper layer,the hierarchical surface showed obvious adhesion resistance to dead bacterial cells and notably migrated the cytotoxic-ity of exposed polycation after completion of the bactericidal task.As a proof-of-principle demonstration,this self-adaptive hierarchical surface with sensitive bacterial responsiveness and biocompatibility showed great potential in combating hernia mesh-related infection.This work provides a promising and universal strategy for the on-demand prevention of medical device-associated infections.展开更多
Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. S...Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. Surface-initiated ringopening polymerization(SI-ROP) of α-amino acid N-carboxyanhydrides represents a powerful and versatile strategy to generate polypeptide brushes. This review is an attempt to capture the state-of-the-art in this field and highlights the latest developments in several selected areas. In addition to presenting an overview of the synthetic methods that have been used to generate polypeptide brushes via SI-ROP, this article will discuss the preparation of patterned polypeptide brushes, the conformational properties of surface-tethered polypeptides, ways to control chain orientation at surfaces as well as properties and applications of these thin polymer films.展开更多
By employing molecular theory, we systematically investigate the shift of solubility of poly(N-isopropylacrylamide)(PNIPAM) brushes in sodium halide solutions. After considering PNIPAM–water hydrogen bonds, water...By employing molecular theory, we systematically investigate the shift of solubility of poly(N-isopropylacrylamide)(PNIPAM) brushes in sodium halide solutions. After considering PNIPAM–water hydrogen bonds, water–anion hydrogen bonds, and PNIPAM–anion bonds and their explicit coupling to the PNIPAM conformations, we find that increasing temperature lowers the solubility of PNIPAM, and results in a collapse of the layer at high enough temperatures. The combination of the three types of bonds would yield a decrease in the solubility of PNIPAM following the Hofmeister series: Na Cl>Na Br>Na I. PNIPAM–water hydrogen bonds are affected by water–anion hydrogen bonds and PNIPAM–anion bonds. The coupling of polymer conformations and the competition among the three types of bonds are essential for describing correctly a decrease in the solubility of PNIPAM brushes, which is determined by the free energy associated with the formation of the three types of bonds. Our results agree well with the experimental observations, and would be very important for understanding the shift of the lower critical solution temperature of PNIPAM brushes following the Hofmeister series.展开更多
Road sweeping is an essential service that has to be conducted for public health,as well as aesthetic purposes.In many countries,sweeping vehicles are used for this activity.They usually comprise a gutter brush that s...Road sweeping is an essential service that has to be conducted for public health,as well as aesthetic purposes.In many countries,sweeping vehicles are used for this activity.They usually comprise a gutter brush that sweeps the debris that is located in the road gutter.This work studies the performance of two kinds of gutter brushes:a cutting brush and a flicking(F128)brush.This is carried out by means of a 3-D dynamic,nonlinear Finite Element(FE)brush model developed by the authors.In this model,inertia forces are applied to the bristle,and its clamped end is fixed.Consequently,the surface(road)is rotated,translated,and raised.Bristle-road interaction is modelled as flexible-to-rigid contact.In particular,the aim of this article is to compare the performance of a conventional brush and a brush rotating at variable speed.As brushes normally work tilted,FE analyses are carried out for tilted cutting and F128 brushes,rotating at speeds that fluctuate at different frequencies.It is concluded that brush oscillations have a significant effect on bristle tip velocities and bristle-road forces.Also,at certain frequencies,oscillations seem to improve sweeping performance of the F128 brush.However,they do not appear to improve significantly the performance of the cutting brush.展开更多
In this work,we investigate the effects of thiocyanate anions on the switching and the structure of poly(Nisopropylacrylamide)(PNIPAM)brushes using a molecular theory.Our model takes into consideration the PNIPAM–ani...In this work,we investigate the effects of thiocyanate anions on the switching and the structure of poly(Nisopropylacrylamide)(PNIPAM)brushes using a molecular theory.Our model takes into consideration the PNIPAM–anion bonds,the electrostatic effects and their explicit coupling to the PNIPAM conformations.It is found that at low thiocyanate anion concentration,as the anion concentration of thiocyanate increases,thiocyanate anions are more associated with PNIPAM chains through the PNIPAM–anion bonds,which contributes to stronger electrostatic repulsion and leads to an increase of lower critical solution temperature(LCST).By analyzing the average volume fractions of PNIPAM brushes,it is found that the PNIPAM brush presents a plateau structure.Our results show that the thiocyanate anions promote phase segregation due to the PNIPAM–anion bonds and the electrostatic effect.According to our model,the reduction of LCST can be explained as follows:at high thiocyanate anion concentration,with the increase of thiocyanate concentration,more ion bindings occurring between thiocyanate anions and PNIPAM chains will result in the increase of the hydrophobicity of PNIPAM chains;when the increase of electrostatic repulsion is insufficient to overcome the hydrophobic interaction of PNIPAM chains,it will lead to the reduction of brush height and LCST at high thiocyanate anion concentration.Our theoretical results are consistent with the experimental observations,and provide a fundamental understanding of the effects of thiocyanate on the LCST of PNIPAM brushes.展开更多
This contribution reports the immobilization of polyoxometalate(POM)into poly(4-vinyl pyridine)(P4 VP)brushes and the controlled reduction of silver ions,in-situ generating metal nanoparticles in the brushes.P4 VP bru...This contribution reports the immobilization of polyoxometalate(POM)into poly(4-vinyl pyridine)(P4 VP)brushes and the controlled reduction of silver ions,in-situ generating metal nanoparticles in the brushes.P4 VP brushes were straightforwardly created by UV-assisted photopolymerization of 4-vinyl pyridine(4VP)on silicon or glass substrates.Phosphotungstic acid(H3 PW12 O40),one of the most widely used Keggin-type POM was anchored onto these pyridine moieties through electrostatic interaction,leading to the P4 VP/POM hybrid brushes.The immobilized POM was further reduced to heteropolyblue,which could be used to generate silver nanoparticles in a controlled fashion.AFM,UV-vis and IR characterization indicate that P4 VP brushes not only provide an efficient platform in the controlled preparation of Ag nanoparticles,but also efficiently disperse and stabilize POM,thus preventing the aggregation of the generated Ag nanoparticles.展开更多
Langevin dynamics simulations have been performed to investigate the response of bi-disperse and strong polyacid chains grafted on an electrode to electric fields generated by opposite surface charges on the polyelect...Langevin dynamics simulations have been performed to investigate the response of bi-disperse and strong polyacid chains grafted on an electrode to electric fields generated by opposite surface charges on the polyelectrolyte (PE)-grafted electrode and a second parallel electrode. Simulation results clearly show that, under a negative external electric field, the longer grafted PE chains are more strongly stretched than the shorter ones in terms of the relative change in their respective brush heights. Whereas under a positive external electric field, the grafted shorter chains collapse more significantly than the longer ones. It was found that, under a positive external electric field, the magnitude of the total electric force acting on one shorter PE chain is larger than that on one longer PE chain, or vice versa. The effects of smeared and discrete charge distributions of grafted PE chains on the response of PE brushes to external electric fields were also examined.展开更多
Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated...Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated PMOXA and SH-terminated PDMAEMA onto polydopamine-anchored substrates.The mixed-brush coating was characterized by variable-angle spectroscopic ellipsometry,X-ray photoelectron spectroscopy,Fourier transform infrared spectroscopy,zeta potential measurements,water contact angle,and atomic force microscopy.The mixed brushes showed tunable surface charge,wettability,and surface roughness,depending on the degree of PDMAEMA swelling under varying pH and ionic strength(Ⅰ).Then the adsorption behaviors of pepsin,bovine serum albumin(BSA),γ-globulin,and lysozyme,four very different proteins with regard to isoelectric point,on the mixed brushes coating were studied by using fluorescence microscopy and surface plasmon resonance.When the chain length of PDMAEMA was about twice as long as PMOXA,the mixed brushes not only had high adsorption capacity for pepsin,BSA,and y-globulin but also had a desorption efficiency of 86.9%,87.1%,and 93.5%,respectively.It is explained that electrostatic attraction between the protonated PDMAEMA and positively charged acidic proteins(pepsin and BSA,whose isoelectric points were below the pK_(a) of PDMAEMA)would drive the intensive adsorption(at pH 3,I=10^(-3)mol·L^(-1)for pepsin,and pH 5,I=10^(-5)mol·L^(-1)for BSA),while desorption was dominated by the hydrophilic PMOXA when PDMAEMA was shrinking(at pH 7,I=10^(-1)mol·L^(-1)for pepsin,and pH 9,I=10^(-1)mol·L^(-1)for BSA).Furthermore,the isoelectric precipitation led to the adsorption of neutral protein(γ-globulin,whose isoelectric point was near the pK_a of PDMAEMA)at pH 7,I=10^(-5)mol·L^(-1),while electrostatic repulsion and antifouling PMOXA triggered the desorption of y-globulin at pH 3,I-10^(-1)mol·L^(-1).However,alkaline protein(lysozyme,whose isoelectric point was higher than the pK_(a) of PDMAEMA)exhibited slight adsorption on PMOXA/PDMAEMA mixed brushes under test conditions,regardless of whether PMOXA or PDMAEMA occupied the outermost layer.The antibacterial property of the mixed brushes against Escherichia coli was investigated.PMOXA/PDMAEMA mixed brushes showed significant bactericidal activity at pH 3,I=10^(-3)mol·L^(-1),while the rinse of pH 9,I=10^(-1)mol·L^(-1)solution could remove most of the residual bacteria.This work not only enables controlled adsorption of proteins with different isoelectric points but also ensures that the surface of the coating is minimized from bacterial contamination.展开更多
The self-consistent field theory has been employed to numerically study the response of bi-disperse flexible polyelectrolyte (PE) brushes grafted on an electrode to electric fields generated by opposite surface char...The self-consistent field theory has been employed to numerically study the response of bi-disperse flexible polyelectrolyte (PE) brushes grafted on an electrode to electric fields generated by opposite surface charges on the PE-grafted electrode and a second parallel electrode. The numerical study reveals that, under a positive external electric field, the shorter and negatively charged PE chains are more responsive than the longer PE chains in terms of the relative changes in their respective brush heights. Whereas under a negative external electric field, the opposite was observed. The total electric force on the grafted PE chains was calculated and it was found that, under a positive external electric field, the magnitude of the total electric force acting on one shorter PE chain is larger than that on one longer PE chain, or vice versa. The underlying mechanism was unraveled through analyzing the total electric field across the two oppositely charged electrodes.展开更多
The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA (Surface Forces Apparatus) the authors measured forc...The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA (Surface Forces Apparatus) the authors measured force-distance profiles of poly (isoprene)-poly (acrylic acid) block copolymers adsorbed on mica. Also by Atomic Force Microscopy the authors captured single polyelectrolyte molecule adsorbed on a surface. The effect of salt concentration (Cs) and pH upon the height of the brush layers was explored mainly by measuring the forces between two adsorbed polyelectrolyte brushes. At pH = 4 our results are in good agreement with the scaling prediction L0 ∝Cs-1/3 Changing the pH from 4 to 10 causes a remarkable swelling of the polymer layer, but only a weak dependence on salt concentration was detected at the higher pH. This can be attributed to the degree of dissociation, which depends on the local pH value. At low pH the polyelectrolyte chains have a low charge density, while on increasing the pH the degree of dissociation rises, and the increased charge density is followed by swelling of the adsorbed layer. The local concentration of ions in the brush is now greater than that of pH = 4 and approximately equivalent to 0.3 M. So the swelling is only weakly dependent on salt concentration in the range 0.01-1.0 M. The results demonstrate the tunable nature of such self-assembled polyelectroiyte brushes whose height and range of interactions, can be systematically controlled by adjusting the pH and ionic strength of the medium.展开更多
Denzel Washington was out with friends whena homeless man asked him for money. The actor’sentourage ignored the beggar, but Washington handedhim a $100 bill. According to The Star, the man began to cry, then grabbed ...Denzel Washington was out with friends whena homeless man asked him for money. The actor’sentourage ignored the beggar, but Washington handedhim a $100 bill. According to The Star, the man began to cry, then grabbed a passerby and chokedout, “Will Smith just gave me a hundred bucks!”展开更多
Implant-related infection is one of the key concerns in clinical medicine, so the modification of titanium to inhibit bacterial adhesion and support osteoblast cell attachment is important. In this article, two strate...Implant-related infection is one of the key concerns in clinical medicine, so the modification of titanium to inhibit bacterial adhesion and support osteoblast cell attachment is important. In this article, two strategies were used to examine the above effects. First, modification of titanium via surface-initiated atom transfer radical polymerization(ATRP) was performed. The surface of the titanium was activated initially by a silane coupling agent. Well-defined polymer brushes of poly(ethylene glycol) methacrylate were successfully tethered on the silane-coupled titanium surface to form hydration shell to examine the anti-fouling effect. Second, functionalization of the Ti-PEG surface with RGD was performed to examine the anti-bacterial adhesion and osteoblast cell attachment ability. The chemical composition of modified titanium surfaces was characterized by X-ray photoelectron spectroscopy(XPS). Changes in surface hydrophilicity and hydrophobicity were characterized by static water contact angle measurements. Results indicated that PEG-RGD brushes were successfully tethered on the titanium surface. And anti-bacterial adhesion ability and osteoblast cell attachment ability were confirmed by fluorescence microscopy and scanning electron microscopy. Results indicated that PEG can inhibit both bacterial adhesion and osteoblast cell attachment, while PEG-RGD brushes can not only inhibit bacterial adhesion but also promote osteoblast cell attachment.展开更多
In the past, many Chinese artists have beenafraid they would be criticized for lagging behindthe world in their conceptions. They are eager todo something unconventional or unorthodox. Theiractions are very similar wi...In the past, many Chinese artists have beenafraid they would be criticized for lagging behindthe world in their conceptions. They are eager todo something unconventional or unorthodox. Theiractions are very similar with the trend Liu展开更多
Gram-negative bacteria can cause serious infections and are well known problems in biomedical practices. Biofilms of gramnegative bacteria are notorious for their frequently encountered resistance toward antibiotics. ...Gram-negative bacteria can cause serious infections and are well known problems in biomedical practices. Biofilms of gramnegative bacteria are notorious for their frequently encountered resistance toward antibiotics. We demonstrate that α/β chimeric polypeptide molecular brush (α/β CPMB) exerts potent activities against antibiotic-resistant gram-negative bacteria. MTT viability assay, bacterial colony counting, and live/dead staining all indicate that α/β CPMB not only inhibits biofilm formation of gram-negative Pseudomonas aeruginosa and Acinetobacter baumannii, but also effectively disrupts mature biofllms that are highly resistant to one of the most active antibiotics-colistin. The superior antibacterial performance of the α/β CPMB implies its potential topical applications in treating biofilms.展开更多
Block copolymer lithography is emerging as one of the leading technologies for patteming nanoscale dense features. In almost all potential applications of this technology, control over the orientation of cylindrical a...Block copolymer lithography is emerging as one of the leading technologies for patteming nanoscale dense features. In almost all potential applications of this technology, control over the orientation of cylindrical and lamellar domains is required for pattern transfer from the block copolymer film. This review highlights the state-of-art development of brushes to modify the substrates to control the assembly behaviors of block copolymers in films. Selected important contributions to the development of self-assembled monolayers, polymer brushes and mats, and chemically patterned brushes are discussed.展开更多
基金supported by the National Natural Science Foundation of China (No.51178451,51138009)
文摘Biological risks of bioaerosols emitted from wastewater treatment processes have attracted wide attention in the recent years. However, the culture-based analysis method has been mostly adopted for detecting the bacterial community in bioaerosols, which may result in the underestimation of total microorganism concentration as not all microorganisms are cultivable. In this study, oligonucleotide fingerprinting of 16S rRNA genes was applied to reveal the composition and structure of the bacterial community in bioaerosols from an Orbal oxidation ditch in a Beijing wastewater treatment plant (WWTP). Bioaerosols were collected at different distances from the aerosol source, rotating brushes, and the sampling height was 1.5 m which is the common respiratory height of a human being. The bacterial communities of bioaerosols were diverse, and the lowest bacterial diversity was found at the sampling site just after the rotating brush rotating brush. A large proportion of bacteria in bioaerosols were affiliated with Proteobacteria and Bacteroidetes. Numerous bacteria present in the bioaerosols also emerged in water, indicating that the bacterial community in the bioaerosols was related to that of the aerosols' sources. The forced aeration of rotating brushes brought about observably distinct bacterial communities between sampling sites situated before and after the rotating brush. Isolation sources of closest relatives in bioaerosols clone libraries were associated with the aqueous environment in the WWTP. Common potential pathogens in bioaerosols as well as those not reported in previous research were also analyzed in this study. Measures should be adopted to reduce the emission of bioaerosols and prevent their exposure to workers.
基金financially supported by the National Natural Science Foundation of China(Nos.21264016 and 11265015)the General Foundation of Yi Li Normal University(No.2013YSYB17)
文摘A theoretical investigation on the pH-induced switching of mixed polyelectrolyte brushes was performed by using a molecular theory. The results indicate that the switching properties of mixed polyelectrolyte brushes are dependent on the pH values. At low pH, negatively charged chains adopt a compact conformation on the bottom of the brush while positively charged chains are highly stretched away from the surface. At high pH values, the inverse transformation takes place. The role of pH determining the polymer chains conformation and charge behavior of mixed polyelectrolyte brushes was analyzed. It is found that there exists a mechanism for reducing strong electrostatic repulsions: stretching of the chains. The H+ and OH- units play a more important role as counterions of the charged polymers do. The collapse of the polyelectrolyte chains for different pH values could be attributed to the screening of the electrostatic interactions and the counterion-mediated attractive interaction along the chains.
基金financially supported by the National Natural Science Foundation of China(No.51273063 and 51003028)the Fundamental Research Funds for the Central Universities+1 种基金the Higher School Specialized Research Fund for the Doctoral Program(No.20110074110003)111 Project Grant(No.B08021)
文摘Spherical polyelectrolyte brushes (SPBs) consisting of polystyrene (PS) core and poly(2-aminoethyl methacrylate hydrochloride) (PAEMH) shell were prepared by photo-emulsion polymerization. Au nanoparticles (Au-NPs) with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.
基金financially by the National Natural Science Foundation of China(No.21004021)the Fundamental Research Funds for the Central Universitiesthe High School Specialized Research Fund for the Doctoral Program(No.20110074110003)
文摘Nano-sized spherical polymer brushes (SPBs) consisting of both a polystyrene (PS) core and a brush shell of poly(acrylic acid) (PAA), poly(N-acrylcysteamine) (PSH), or poly(N-acrylcysteamine-co-acrylic acid) (P(SH-co-AA)), were prepared by photo-emulsion polymerization. The core-shell structure was observed by dynamic light scattering and transmission electron microscopy. Due to the strengthened Donnan effect, the PAA brush can adsorb heavy metal ions. Effects of the contact time, thickness of PAA brush and pH value on the adsorption results were investigated. Due to the coordination between the mercapto groups and heavy metal ions as well as the electrostatic interactions, SPBs with mercapto groups are capable to remove heavy metal ions selectively from aqueous solutions. The order of adsorption capacity of the heavy metal ions by SPBs with mercapto groups is: Hg2+ ≈ Au3+ 〉 Pb2+ 〉 CH2+ 〉 Ni2+. The adsorbed heavy metal ions can be eluted from SPB by aqueous HCI solution, and the SPBs can be recovered. After three regenerations the recovered SPBs still maintain their adsorption capacity.
基金financially supported by PULEAD Technology Industry Co.,Ltd.the National Natural Science Foundation of China(Nos.21771018,21875004)。
文摘Polymer electrolytes a re essential for next-gene ration lithium batteries because of their excellent safety record.However,low ionic conductivity is the main obstacle restricting their commercial application.Composites with nanoparticles are a promising route to overcome this obstacle.In this work,lithium polystyrene sulfonate brushes(LiPSS)is anchored to silicon dioxide nanoparticles with chemical bonding using atom transfer radial polymerization(SI-ATRP).The composite polymer electrolytes are made by mixing vinylene carbonate and nanoparticles via a facile in situ polymerization process.The ionic conductivity of composite polymer electrolytes is improved to 7.2×10^-4 S/cm at room temperature,which is attributed to the low degree of crystallinity of polymer electrolyte and the fast ion transport on the surfaces of polymer brush layers that act as a conductive network.The composite polymer electrolytes show a wide electrochemical window of approximately 4.5 V vs.Li^+/Li and excellent cycling performance retention of approximately 95%after 100 cycles at ambient temperature.The results also prove that surface groups of ceramic na noparticles are an important way to increase the electrochemical properties of composite polymer electrolytes.
基金supported by the National Natural Science Foundation of China(No.51873213)the Natural Science Foundation of Jilin Province(No.20210101385JC)+1 种基金the High-Tech Research&Development Program of CAS-WEGO Groupthe Major Science and Technology Innovation Project of Shandong Province(No.2019JZZY011105).
文摘Hierarchical polymer brushes have been considered as an effective and promising method for preventing implant-associated infections via multiple antibacterial mechanisms.Herein,a bacterial phosphatase re-sponsive surface with hierarchical zwitterionic structures was developed for timely dealing with the poly-meric implant-associated bacterial infection.The hierarchical polymeric architecture was subtly realized on model polypropylene(PP)substrate by sequential photo living grafting of poly(2-(dimethylamino)ethyl methacrylate(PDMAEMA)bottom layer and zwitterionic poly(sulfobetaine methacrylate)(PSBMA)upper layer,followed by the conversion of the PDMAEMA into the zwitterionic structure via succes-sive quaternization and phosphorylation reactions.Owing to shielding the bottom polycations,the hi-erarchical zwitterionic polymer brushes guaranteed the surface with the optimal biocompatibility under the normal physiological environment.Once bacteria are invaded,the surface bactericidal activity of the bottom layer can be rapidly and automatically activated owing to the transition triggered by bacterial phosphatase from zwitterion to polycation.Additionally,ameliorated by the upper layer,the hierarchical surface showed obvious adhesion resistance to dead bacterial cells and notably migrated the cytotoxic-ity of exposed polycation after completion of the bactericidal task.As a proof-of-principle demonstration,this self-adaptive hierarchical surface with sensitive bacterial responsiveness and biocompatibility showed great potential in combating hernia mesh-related infection.This work provides a promising and universal strategy for the on-demand prevention of medical device-associated infections.
基金financially supported by the Sino-Swiss Science and Technology Cooperation(No.EG41-092011)as well as the Chinese Academy of Sciences(Visiting Professorship for Senior International Scientists to H.A.K.)
文摘Polypeptide brushes are attractive platforms to generate functional and responsive interfaces that are of potential interest due to their possible biodegradability, biocompatibility and tunable secondary structures. Surface-initiated ringopening polymerization(SI-ROP) of α-amino acid N-carboxyanhydrides represents a powerful and versatile strategy to generate polypeptide brushes. This review is an attempt to capture the state-of-the-art in this field and highlights the latest developments in several selected areas. In addition to presenting an overview of the synthetic methods that have been used to generate polypeptide brushes via SI-ROP, this article will discuss the preparation of patterned polypeptide brushes, the conformational properties of surface-tethered polypeptides, ways to control chain orientation at surfaces as well as properties and applications of these thin polymer films.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21264016,11464047,and 21364016)the Joint Funds of Xinjiang Natural Science Foundation,China(Grant No.2015211C298)
文摘By employing molecular theory, we systematically investigate the shift of solubility of poly(N-isopropylacrylamide)(PNIPAM) brushes in sodium halide solutions. After considering PNIPAM–water hydrogen bonds, water–anion hydrogen bonds, and PNIPAM–anion bonds and their explicit coupling to the PNIPAM conformations, we find that increasing temperature lowers the solubility of PNIPAM, and results in a collapse of the layer at high enough temperatures. The combination of the three types of bonds would yield a decrease in the solubility of PNIPAM following the Hofmeister series: Na Cl>Na Br>Na I. PNIPAM–water hydrogen bonds are affected by water–anion hydrogen bonds and PNIPAM–anion bonds. The coupling of polymer conformations and the competition among the three types of bonds are essential for describing correctly a decrease in the solubility of PNIPAM brushes, which is determined by the free energy associated with the formation of the three types of bonds. Our results agree well with the experimental observations, and would be very important for understanding the shift of the lower critical solution temperature of PNIPAM brushes following the Hofmeister series.
文摘Road sweeping is an essential service that has to be conducted for public health,as well as aesthetic purposes.In many countries,sweeping vehicles are used for this activity.They usually comprise a gutter brush that sweeps the debris that is located in the road gutter.This work studies the performance of two kinds of gutter brushes:a cutting brush and a flicking(F128)brush.This is carried out by means of a 3-D dynamic,nonlinear Finite Element(FE)brush model developed by the authors.In this model,inertia forces are applied to the bristle,and its clamped end is fixed.Consequently,the surface(road)is rotated,translated,and raised.Bristle-road interaction is modelled as flexible-to-rigid contact.In particular,the aim of this article is to compare the performance of a conventional brush and a brush rotating at variable speed.As brushes normally work tilted,FE analyses are carried out for tilted cutting and F128 brushes,rotating at speeds that fluctuate at different frequencies.It is concluded that brush oscillations have a significant effect on bristle tip velocities and bristle-road forces.Also,at certain frequencies,oscillations seem to improve sweeping performance of the F128 brush.However,they do not appear to improve significantly the performance of the cutting brush.
基金Project supported by the Joint Funds of Xinjiang Natural Science Foundation(Grant No.2019D01C333)the National Natural Science Foundation of China(Grant Nos.11847610 and 21764015)the National Basic Research Program of China(Grant No.2015CB857100)
文摘In this work,we investigate the effects of thiocyanate anions on the switching and the structure of poly(Nisopropylacrylamide)(PNIPAM)brushes using a molecular theory.Our model takes into consideration the PNIPAM–anion bonds,the electrostatic effects and their explicit coupling to the PNIPAM conformations.It is found that at low thiocyanate anion concentration,as the anion concentration of thiocyanate increases,thiocyanate anions are more associated with PNIPAM chains through the PNIPAM–anion bonds,which contributes to stronger electrostatic repulsion and leads to an increase of lower critical solution temperature(LCST).By analyzing the average volume fractions of PNIPAM brushes,it is found that the PNIPAM brush presents a plateau structure.Our results show that the thiocyanate anions promote phase segregation due to the PNIPAM–anion bonds and the electrostatic effect.According to our model,the reduction of LCST can be explained as follows:at high thiocyanate anion concentration,with the increase of thiocyanate concentration,more ion bindings occurring between thiocyanate anions and PNIPAM chains will result in the increase of the hydrophobicity of PNIPAM chains;when the increase of electrostatic repulsion is insufficient to overcome the hydrophobic interaction of PNIPAM chains,it will lead to the reduction of brush height and LCST at high thiocyanate anion concentration.Our theoretical results are consistent with the experimental observations,and provide a fundamental understanding of the effects of thiocyanate on the LCST of PNIPAM brushes.
基金The financial support of this work by Department of Science and Technology of Jilin Province(Nos.20180101196JC and20180101170JC)
文摘This contribution reports the immobilization of polyoxometalate(POM)into poly(4-vinyl pyridine)(P4 VP)brushes and the controlled reduction of silver ions,in-situ generating metal nanoparticles in the brushes.P4 VP brushes were straightforwardly created by UV-assisted photopolymerization of 4-vinyl pyridine(4VP)on silicon or glass substrates.Phosphotungstic acid(H3 PW12 O40),one of the most widely used Keggin-type POM was anchored onto these pyridine moieties through electrostatic interaction,leading to the P4 VP/POM hybrid brushes.The immobilized POM was further reduced to heteropolyblue,which could be used to generate silver nanoparticles in a controlled fashion.AFM,UV-vis and IR characterization indicate that P4 VP brushes not only provide an efficient platform in the controlled preparation of Ag nanoparticles,but also efficiently disperse and stabilize POM,thus preventing the aggregation of the generated Ag nanoparticles.
基金supported by the National Natural Science Foundation of China(Grant No.21374052)
文摘Langevin dynamics simulations have been performed to investigate the response of bi-disperse and strong polyacid chains grafted on an electrode to electric fields generated by opposite surface charges on the polyelectrolyte (PE)-grafted electrode and a second parallel electrode. Simulation results clearly show that, under a negative external electric field, the longer grafted PE chains are more strongly stretched than the shorter ones in terms of the relative change in their respective brush heights. Whereas under a positive external electric field, the grafted shorter chains collapse more significantly than the longer ones. It was found that, under a positive external electric field, the magnitude of the total electric force acting on one shorter PE chain is larger than that on one longer PE chain, or vice versa. The effects of smeared and discrete charge distributions of grafted PE chains on the response of PE brushes to external electric fields were also examined.
基金the financial support of the National Natural Science Foundation of China(21674102)。
文摘Herein,binary mixed brushes consisting of poly(2-methyl-2-oxazoline)(PMOXA)and poly(2-(dimethylamine)ethyl methacrylate)(PDMAEMA)with different chain lengths were fabricated by successive grafting of NH_(2)-terminated PMOXA and SH-terminated PDMAEMA onto polydopamine-anchored substrates.The mixed-brush coating was characterized by variable-angle spectroscopic ellipsometry,X-ray photoelectron spectroscopy,Fourier transform infrared spectroscopy,zeta potential measurements,water contact angle,and atomic force microscopy.The mixed brushes showed tunable surface charge,wettability,and surface roughness,depending on the degree of PDMAEMA swelling under varying pH and ionic strength(Ⅰ).Then the adsorption behaviors of pepsin,bovine serum albumin(BSA),γ-globulin,and lysozyme,four very different proteins with regard to isoelectric point,on the mixed brushes coating were studied by using fluorescence microscopy and surface plasmon resonance.When the chain length of PDMAEMA was about twice as long as PMOXA,the mixed brushes not only had high adsorption capacity for pepsin,BSA,and y-globulin but also had a desorption efficiency of 86.9%,87.1%,and 93.5%,respectively.It is explained that electrostatic attraction between the protonated PDMAEMA and positively charged acidic proteins(pepsin and BSA,whose isoelectric points were below the pK_(a) of PDMAEMA)would drive the intensive adsorption(at pH 3,I=10^(-3)mol·L^(-1)for pepsin,and pH 5,I=10^(-5)mol·L^(-1)for BSA),while desorption was dominated by the hydrophilic PMOXA when PDMAEMA was shrinking(at pH 7,I=10^(-1)mol·L^(-1)for pepsin,and pH 9,I=10^(-1)mol·L^(-1)for BSA).Furthermore,the isoelectric precipitation led to the adsorption of neutral protein(γ-globulin,whose isoelectric point was near the pK_a of PDMAEMA)at pH 7,I=10^(-5)mol·L^(-1),while electrostatic repulsion and antifouling PMOXA triggered the desorption of y-globulin at pH 3,I-10^(-1)mol·L^(-1).However,alkaline protein(lysozyme,whose isoelectric point was higher than the pK_(a) of PDMAEMA)exhibited slight adsorption on PMOXA/PDMAEMA mixed brushes under test conditions,regardless of whether PMOXA or PDMAEMA occupied the outermost layer.The antibacterial property of the mixed brushes against Escherichia coli was investigated.PMOXA/PDMAEMA mixed brushes showed significant bactericidal activity at pH 3,I=10^(-3)mol·L^(-1),while the rinse of pH 9,I=10^(-1)mol·L^(-1)solution could remove most of the residual bacteria.This work not only enables controlled adsorption of proteins with different isoelectric points but also ensures that the surface of the coating is minimized from bacterial contamination.
基金financially supported by the National Natural Science Foundation of China(No.21374052)the support from K.C.Wong Magna Fund in Ningbo University
文摘The self-consistent field theory has been employed to numerically study the response of bi-disperse flexible polyelectrolyte (PE) brushes grafted on an electrode to electric fields generated by opposite surface charges on the PE-grafted electrode and a second parallel electrode. The numerical study reveals that, under a positive external electric field, the shorter and negatively charged PE chains are more responsive than the longer PE chains in terms of the relative changes in their respective brush heights. Whereas under a negative external electric field, the opposite was observed. The total electric force on the grafted PE chains was calculated and it was found that, under a positive external electric field, the magnitude of the total electric force acting on one shorter PE chain is larger than that on one longer PE chain, or vice versa. The underlying mechanism was unraveled through analyzing the total electric field across the two oppositely charged electrodes.
文摘The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA (Surface Forces Apparatus) the authors measured force-distance profiles of poly (isoprene)-poly (acrylic acid) block copolymers adsorbed on mica. Also by Atomic Force Microscopy the authors captured single polyelectrolyte molecule adsorbed on a surface. The effect of salt concentration (Cs) and pH upon the height of the brush layers was explored mainly by measuring the forces between two adsorbed polyelectrolyte brushes. At pH = 4 our results are in good agreement with the scaling prediction L0 ∝Cs-1/3 Changing the pH from 4 to 10 causes a remarkable swelling of the polymer layer, but only a weak dependence on salt concentration was detected at the higher pH. This can be attributed to the degree of dissociation, which depends on the local pH value. At low pH the polyelectrolyte chains have a low charge density, while on increasing the pH the degree of dissociation rises, and the increased charge density is followed by swelling of the adsorbed layer. The local concentration of ions in the brush is now greater than that of pH = 4 and approximately equivalent to 0.3 M. So the swelling is only weakly dependent on salt concentration in the range 0.01-1.0 M. The results demonstrate the tunable nature of such self-assembled polyelectroiyte brushes whose height and range of interactions, can be systematically controlled by adjusting the pH and ionic strength of the medium.
文摘Denzel Washington was out with friends whena homeless man asked him for money. The actor’sentourage ignored the beggar, but Washington handedhim a $100 bill. According to The Star, the man began to cry, then grabbed a passerby and chokedout, “Will Smith just gave me a hundred bucks!”
文摘Implant-related infection is one of the key concerns in clinical medicine, so the modification of titanium to inhibit bacterial adhesion and support osteoblast cell attachment is important. In this article, two strategies were used to examine the above effects. First, modification of titanium via surface-initiated atom transfer radical polymerization(ATRP) was performed. The surface of the titanium was activated initially by a silane coupling agent. Well-defined polymer brushes of poly(ethylene glycol) methacrylate were successfully tethered on the silane-coupled titanium surface to form hydration shell to examine the anti-fouling effect. Second, functionalization of the Ti-PEG surface with RGD was performed to examine the anti-bacterial adhesion and osteoblast cell attachment ability. The chemical composition of modified titanium surfaces was characterized by X-ray photoelectron spectroscopy(XPS). Changes in surface hydrophilicity and hydrophobicity were characterized by static water contact angle measurements. Results indicated that PEG-RGD brushes were successfully tethered on the titanium surface. And anti-bacterial adhesion ability and osteoblast cell attachment ability were confirmed by fluorescence microscopy and scanning electron microscopy. Results indicated that PEG can inhibit both bacterial adhesion and osteoblast cell attachment, while PEG-RGD brushes can not only inhibit bacterial adhesion but also promote osteoblast cell attachment.
文摘In the past, many Chinese artists have beenafraid they would be criticized for lagging behindthe world in their conceptions. They are eager todo something unconventional or unorthodox. Theiractions are very similar with the trend Liu
基金financially supported by the National Natural Science Foundation of China (Nos. 21574038, 21774031, and 21861162010)the Natural Science Foundation of Shanghai (No. 18ZR1410300)+2 种基金the “Eastern Scholar Professorship” from Shanghai local government (No. TP2014034)the national special fund for State Key Laboratory of Bioreactor Engineering (No. 2060204)the Fundamental Research Funds for the Central Universities (No. 22221818014)
文摘Gram-negative bacteria can cause serious infections and are well known problems in biomedical practices. Biofilms of gramnegative bacteria are notorious for their frequently encountered resistance toward antibiotics. We demonstrate that α/β chimeric polypeptide molecular brush (α/β CPMB) exerts potent activities against antibiotic-resistant gram-negative bacteria. MTT viability assay, bacterial colony counting, and live/dead staining all indicate that α/β CPMB not only inhibits biofilm formation of gram-negative Pseudomonas aeruginosa and Acinetobacter baumannii, but also effectively disrupts mature biofllms that are highly resistant to one of the most active antibiotics-colistin. The superior antibacterial performance of the α/β CPMB implies its potential topical applications in treating biofilms.
基金financially supported by the National Natural Science Foundation of China(Nos.51173181 and 51373166)“The Hundred Talents Program”from the Chinese Academy of Sciences and the International S&T Cooperation Program from Department of Science and Technology of Jilin Province(No.20160414032GH)
文摘Block copolymer lithography is emerging as one of the leading technologies for patteming nanoscale dense features. In almost all potential applications of this technology, control over the orientation of cylindrical and lamellar domains is required for pattern transfer from the block copolymer film. This review highlights the state-of-art development of brushes to modify the substrates to control the assembly behaviors of block copolymers in films. Selected important contributions to the development of self-assembled monolayers, polymer brushes and mats, and chemically patterned brushes are discussed.