Phosphorus(P)is crucial for crop growth.However,in waters,P is considered as contaminant due to its role in causing eutrophication and algae blooms.Therefore,recovering P from wastewater is essential for sustainable P...Phosphorus(P)is crucial for crop growth.However,in waters,P is considered as contaminant due to its role in causing eutrophication and algae blooms.Therefore,recovering P from wastewater is essential for sustainable P management.This study investigated the removal of P from aqueous solutions using bioinspired poly(ethylenimine)-poly(acrylamideco-acrylic acid)(PEI-PAMcoAA)coacervates.In detail,we investigated various parameters affecting P removal,including the ratio of PEI to PAMcoAA(ranging from 1:2 to 3:1,stoichiometry ratio of NH_(2) to COOH),pH(5.0-8.0)of P-containing solutions,initial P concentration(0.05-5 mmol/L),and the addition of calcium(Ca,0.1-5 mmol/L).We found that increasing the PEI:PAMcoAA ratio from1:2 to 3:1 significantly enhanced P removal efficiency,increasing from 47.21%to 95.44%.Under neutral pH conditions without calcium(Ca),PEI-PAMcoAA coacervates demonstrated optimal P removal capabilities(achieving an efficiency of 77.96%)through electrostatic adsorption.In contrast,the addition of Ca under alkaline conditions markedly improved P removal efficiency,increasing it from 64.16%to 82.42%.Detailed analyses of P within the coacervates indicated that Ca facilitates P precipitation and provides additional binding sites.These findings demonstrated that PEI-(Ca)-PAMcoAA coacervates show promise for efficiently removing P,particularly at low P concentrations.After the Premoval,the immobilized P can potentially be reused directly,as P able to be released from the reacted products.Therefore,the reacted coacervates could serve as a non-toxic fertilizer.Given its simplicity,high efficiency,and environmental friendliness,P removal based on bioinspired coacervates represents a low-hanging fruit in the pursuit of sustainable P management.展开更多
The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic environment.Resolving the regulation mechanism is still a challenge.In this work,we designed a s...The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic environment.Resolving the regulation mechanism is still a challenge.In this work,we designed a series of peptides(XXLY)_(6)SSSGSS and studied their complexation and coacervation behavior with single-stranded oligonucleotides.The“X”and“Y”are varied to combine known amounts of charged and non-charged amino acids,together with the introduction of secondary structures and pH responsiveness.Results show that the electrostatic interaction,which is described as charge density,controls both the strength of complexation and the degree of chain relaxation,and thus determines the growth and size of the coacervates.The hydrophobic interaction is prominent when the charges are neutralized.Interestingly,the secondary structures of peptides exhibit profound effect on the morphology of the phases,such as solid phase to liquid phase transition.Our study gains insight into the phase separation under physiological conditions.It is also helpful to create coacervates with desirable structures and functions.展开更多
Significant progress has been made in wet adhesives for low salinity water,but exploration of general ionic adhesives for natural seawater is less developed because the high salinity could weaken interfacial bonding a...Significant progress has been made in wet adhesives for low salinity water,but exploration of general ionic adhesives for natural seawater is less developed because the high salinity could weaken interfacial bonding and shields electrostatic interactions,resulting in adhesion failure.Thus,the design of adhesives for natural seawater represents challenges less resolved.Herein,a cationic polyelectrolyte(PECHIA)containing imidazolacetonitrile unit was explored to prepare adhesives enabled by natural seawater.By combining the ion shielding effect with the“cation-dipole”interactions between PECHIA chains,aqueous solution of the PECHIA underwent coacervation and self-crosslinking in natural seawater,allowing for underwater adhesion to various substrates in seawater.The instantaneous lap-shear and tensile adhesion strengths are 47 and 119 kPa,respectively,while the cured adhesive shows~739 k Pa tensile adhesion in natural seawater.The design of PECHIA enables wet adhesives viable for applications in the diversified scenarios of natural seawater.展开更多
Hexafluoroisopropanol(HFIP)-induced sodium dodecyl sulfate/dodecyltrimethylammonium bromide(SDS/DTAB) catanionic surfactant coacervate extraction method coupled with high performance liquid chromatography(HPLC) was us...Hexafluoroisopropanol(HFIP)-induced sodium dodecyl sulfate/dodecyltrimethylammonium bromide(SDS/DTAB) catanionic surfactant coacervate extraction method coupled with high performance liquid chromatography(HPLC) was used to detect the migration of phthalates from disposable tablewares to drinking water. The concentration factors are larger than 82 and extraction recoveries over 53% for water samples spiked with 100 or 200 ng/m L phthalates. Limit of detection is in the range of 1.0–2.6 ng/m L.Good linearity with correlation coefficients larger than 0.9985 is obtained in the concentration of20–1500 or 40–3000 ng/m L. Relative recoveries are from 82.4% to 123.6% for water samples spiked with30/60, 250/500, and 1500/3000 ng/m L phthalates, respectively. Relative standard deviations(RSDs) are0.4%–7.4% for intraday precision(n = 5) and 0.6%–7.8% for interday precision(n = 3). Four of studied phthalates are found in the drinking water samples prepared from four kinds of tablewares.展开更多
The microstructure of CdI2 thin film grown during vapor-phase deposition was investigated by scanning electron microscopy (SEM). The thin film deposited on Si crystal consists of numerous sunflower-like aggregates. Th...The microstructure of CdI2 thin film grown during vapor-phase deposition was investigated by scanning electron microscopy (SEM). The thin film deposited on Si crystal consists of numerous sunflower-like aggregates. These aggregates display well self-assembly characteristics. The size of Sunflower-like aggregates is between 12 and 44 μm. Each sunflower-like aggregate is surrounded with many adjacent wings-'petals'. The structure of central region of the 'sunflower' is obviously difFerent from that of the 'petal'. Electron spectroscopy for chemical analysis (ESCA) was employed in determining the chemical valence of the thin film. Self-organization efFect is used to explain the coring growth process of CdI2 thin film展开更多
Liquid–liquid phase separation(LLPS)induces the formation of membrane-less droplet-like compartments through the segregation of biomolecules into distinct liquid phases within a solution,without the requirement for a...Liquid–liquid phase separation(LLPS)induces the formation of membrane-less droplet-like compartments through the segregation of biomolecules into distinct liquid phases within a solution,without the requirement for a surrounding lipid bilayer1.These membrane-less droplet-like compartments,which arise from LLPS,possess unique properties and functions essential for cellular organization,biomolecular condensation,and cellular signaling2.展开更多
Recent progress in nanotechnology and synthetic biology has demonstrated the potential of DNA coacervates for biomimetic and biological applications.DNA coacervates are micron-scale,membrane-free,spherical structures ...Recent progress in nanotechnology and synthetic biology has demonstrated the potential of DNA coacervates for biomimetic and biological applications.DNA coacervates are micron-scale,membrane-free,spherical structures formed by liquid-liquid phase separation of DNA materials.They uniquely combine the programmability of DNA with the fluidic properties of coacervates,allowing for controlled modulation of their structures,biomimetic and biological functions,and dynamic behaviors through rational sequence design.This review summarizes methods for the formation of different DNA coacervates and explores their extensive applications in biomimicry,biosensing and therapeutics.Limitations and prospects of DNA coacervates are also discussed.展开更多
Controlled delivery of proteins and other biologics is a growing medium of therapy for diseases previously untreatable.Here we report a self-assembling,tunable vesicle for the controlled delivery of growth factors and...Controlled delivery of proteins and other biologics is a growing medium of therapy for diseases previously untreatable.Here we report a self-assembling,tunable vesicle for the controlled delivery of growth factors and cytokines.Coacervate made of heparin and a biocompatible polycation,PEAD,forms the core of the vesicle;lipids form the membrane of the vesicle.We call this vesicle lipocoacervate(LipCo),which has a high affinity for growth factors and cytokines due to heparin.LipCo is a tunable protein delivery vehicle.The vesicle size is controlled through polymer and salt concentrations.Membrane functionalization enables potential for targeting capabilities with long-term storage through lyophilization.Importantly,the controlled delivery of therapeutics also avoids high toxicity to treated cells in vitro.Here we report on these key principles of LipCo assembly and design.展开更多
Developing an oral in situ-forming hydrogel that targets the inflamed intestine to suppress bleeding ulcers and alleviate intestinal inflammation is crucial for effectively treating ulcerative colitis(UC).Here,inspire...Developing an oral in situ-forming hydrogel that targets the inflamed intestine to suppress bleeding ulcers and alleviate intestinal inflammation is crucial for effectively treating ulcerative colitis(UC).Here,inspired by sandcastle worm adhesives,we proposed a water-immiscible coacervate(EMNs-gel)with a programmed coacervate-to-hydrogel transition at inflammatory sites composed of dopa-rich silk fibroin matrix containing embedded inflammation-responsive core-shell nanoparticles.Driven by intestinal peristalsis,the EMNs-gel can be actuated forward and immediately transform into a hydrogel once contacting with the inflamed intestine to yield strong tissue adhesion,resulting from matrix metalloproteinases(MMPs)-triggered release of Fe3+from embedded nanoparticles and rearrangement of polymer network of EMNs-gel on inflamed intestine surfaces.Extensive in vitro experiments and in vivo UC models confirmed the preferential hydrogelation behavior of EMNs-gel to inflamed intestine surfaces,achieving highly effective hemostasis,and displaying an extended residence time(48 h).This innovative EMNs-gel provides a non-invasive solution that accurately suppresses severe bleeding and improves intestinal homeostasis in UC,showcasing great potential for clinical applications.展开更多
Engineering hydrogels that resemble biological tissues of various lengths via conventional fabrication techniques remains challenging.Three-dimensional(3D)bioprinting has emerged as an advanced approach for constructi...Engineering hydrogels that resemble biological tissues of various lengths via conventional fabrication techniques remains challenging.Three-dimensional(3D)bioprinting has emerged as an advanced approach for constructing complex biomimetic 3D architectures,which are currently restricted by the limited number of available bioinks with high printability,biomimicry,biocompatibility,and proper mechanical properties.Inspired by ubiquitous coacervation phenomena in biology,we present a unique mineral-biopolymer coacervation strategy that enables the hierarchical assembly of nanoclay and recombinant human collagen(RHC).This system was observed to undergo a coacervation transition(liquid‒liquid phase separation)spontaneously.The formed dense phase separated from its supernatant is the coacervate of clay-RHC-rich complexes,where polymer chains are sandwiched between silicate layers.Molecular dynamics simulation was first used to verify and explore the coacervation process.Then,the coacervates were demonstrated to be potential bioinks that exhibited excellent self-supporting and shear-thinning viscoelastic properties.Through extrusion-based printing,the versatility of the bioink was demonstrated by reconstructing the key features of several biological tissues,including multilayered lattice,vascular,nose,and ear-like structures,without the need for precrosslinking operations or support baths.Furthermore,the printed scaffolds were cytocompatible,elicited minimal inflammatory responses,and promoted bone regeneration in calvarial defects.展开更多
Oral ulcers are a common ulcerative injury that occurs in the oral mucosa.When occurring,they can cause mucosal pain and affect eating and communication.The oral cavity,characterized by its moist environment and const...Oral ulcers are a common ulcerative injury that occurs in the oral mucosa.When occurring,they can cause mucosal pain and affect eating and communication.The oral cavity,characterized by its moist environment and constant movement of the lips and tongue,presents challenges for conventional drug delivery systems due to its suboptimal adhesion.Therefore,there is a need for the development of adhesive materials specifically designed for use within the oral cavity.In this research,a sticky coacervate incorporating tea polyphenols(TP)was formulated based on the adhesive properties observed in sandcastle worms.The coacervate is composed of Pluronic F68(F68)and TP,synthesized through the coacervation reaction.The F68-TP coacervates are attached to porcine skin easily.It also reduces bacterial viability and has the ability to clear reactive oxygen species.In animal ulcer models,these coacervates demonstrate anti-inflammatory effects and enhance collagen and muscle fiber synthesis.Overall,these adhesive coacervates with antioxidative and antibacterial properties hold potential as a therapeutic option for oral ulcers in the oral cavity.展开更多
Heart disease is still the leading killer all around the world,and its incidence is expected to increase over the next decade.Previous reports have already shown the role of fibroblast growth factor10(FGF10)in allevia...Heart disease is still the leading killer all around the world,and its incidence is expected to increase over the next decade.Previous reports have already shown the role of fibroblast growth factor10(FGF10)in alleviating heart diseases.However,FGF10 has not been used to treat heart diseases because the free protein has short half-life and low bioactivity.Here,an injectable coacervate was designed to protect growth factor from degradation during delivery and the effects of the FGF10 coacervate were studied using a mice acute myocardial infarction(MI)model.As shown in our echocardiographic results,a single injection of FGF10 coacervate effectively inhibited preserved cardiac contractibility and ventricular dilation when compared with free FGF10 and the saline treatment 6 weeks after MI.It is revealed in histological results that the MI induced myocardial inflammation and fibrosis was reduced after FGF10 coacervate treatment.Furthermore,FGF10 coacervate treatment could improve arterioles and capillaries stabilization through increasing the proliferation of endothelial and mural cells.However,with the same dosage,no statistically significant difference was shown between free FGF10,heparin+FGF10 and saline treatment,especially in long term.On another hand,FGF10 coacervate also increased the expression of cardiac-associated the mRNA(cTnT,Cx43 and α-SMA),angiogenic factors(Ang-1 and VEGFA)and decreased the level of inflammatory factor(tumor necrosis factor-α).The downstream signaling of the FGF10 was also investigated,with the western blot results showing that FGF10 coacervate activated the p-FGFR,PI3K/Akt and ERK1/2 pathways to a more proper level than free FGF10 or heparin+FGF10.In general,it is revealed in this research that one-time injection of FGF10 coacervate sufficiently attenuated MI induced injury when compared with an equal dose of free FGF10 or heparin+FGF10 injection.展开更多
Protecting the skin from UV light irradiation in wet and underwater environments is challenging due to the weak adhesion of existing sunscreen materials but highly desired.Herein we report a polyethyleneimine/thioctic...Protecting the skin from UV light irradiation in wet and underwater environments is challenging due to the weak adhesion of existing sunscreen materials but highly desired.Herein we report a polyethyleneimine/thioctic acid/titanium dioxide(PEI/TA/TiO_(2))coacervate-derived hydrogel with robust,asymmetric,and reversible wet bioadhesion and effective UV-light-shielding ability.The PEI/TA/TiO_(2)complex coacervate can be easily obtained by mixing a PEI solution and TA/TiO_(2)powder.The fluid PEI/TA/TiO_(2)coacervate deposited on wet skin can spread into surface irregularities and subsequently transform into a hydrogel with increased cohesion,thereby establishing interdigitated contact and adhesion between the bottom surface and skin.Meanwhile,the functional groups between the skin and hydrogel can form physical interactions to further enhance bioadhesion,whereas the limited movement of amine and carboxyl groups on the top hydrogel surface leads to low adhesion.Therefore,the coacervate-derived hydrogel exhibits asymmetric adhesiveness on the bottom and top surfaces.Moreover,the PEI/TA/TiO_(2)hydrogel formed on the skin could be easily removed using a NaHCO3 aqueous solution without inflicting damage.More importantly,the PEI/TA/TiO_(2)hydrogel can function as an effective sunscreen to block UV light and prevent UV-induced MMP-9 overexpression,inflammation,and DNA damage in animal skin.The advantages of PEI/TA/TiO_(2)coacervate-derived hydrogels include robust,asymmetric,and reversible wet bioadhesion,effective UV light-shielding ability,excellent biocompatibility,and easy preparation and usage,making them a promising bioadhesive to protect the skin from UV light-associated damage in wet and underwater environments.展开更多
Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are...Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are scarce.Herein,we develop a simple system made of a surfactant(-)-N-dodecylN-methylephedrinium bromide(DMEB)and inorganic salts that is capable of spontaneous formation of vesicles,coacervates,and the reversible transformation between the two states.展开更多
Many functional coacervates have been identified in biological systems,which have attracted widespread interest.Coacervation is a liquid–liquid phase separation(LLPS)process in which a macromolecule-enriched liquid p...Many functional coacervates have been identified in biological systems,which have attracted widespread interest.Coacervation is a liquid–liquid phase separation(LLPS)process in which a macromolecule-enriched liquid phase is formed together with a macromolecule-depleted phase.Bio-inspired coacervates possess excellent features such as underwater delivery,low interface energy,shear thinning,and excellent biocompatibility.They also serve as good delivery platforms for different types of molecules.In this review,we briefly discuss some important extracellular coacervate systems,including mussel adhesives,sandcastle worm glue,squid beak,and tropoelastin.We then provide an overview of the recent development of bio-inspired functional coacervates for various biomedical applications,including medical adhesives,drug delivery,and tissue engineering.Bio-inspired functional coacervates offer a promising material platform for developing new materials for biomedical applications.展开更多
Using sodium laureth sulfate(AES)as reference,the effects of different pH values on the foam properties of four amino acid surfactants(sodium lauroyl sarcosinate,lauroyl alanine,disodium cocoyl glutamate,sodium methyl...Using sodium laureth sulfate(AES)as reference,the effects of different pH values on the foam properties of four amino acid surfactants(sodium lauroyl sarcosinate,lauroyl alanine,disodium cocoyl glutamate,sodium methyl cocoyl taurate)were compared.On the basis,the effects of amino acid surfactants on foam performance,flocculation behavior,hair color protection efficacy and sebum removal capacity were studied when AES was completely or partially replaced by amino acid surfactant,and the correlation between the structure of amino acid surfactant and these properties was discussed.Compared with AES,the foam performance of sodium lauroyl sarcosinate,lauroyl alanine and disodium cocoyl glutamate were significantly affected by pH value,and sodium methyl cocoyl taurate was less affected.The foam stability of shampoo system can be enhanced by the combination of amino acid surfactant,and the foam performance of shampoo system can be significantly improved by the combination of sodium methyl cocoyl taurate.All the four amino acid surfactants can prolong the flocculation time of shampoo,and the effect of disodium cocoyl glutamate was the most obvious.The hair color protection efficacy of disodium cocoyl glutamate and sodium methyl cocoyl taurate were better than AES.The degreasing power of disodium cocoyl glutamate was weaker than that of AES,and the degreasing power of sodium lauroyl sarcosinate,lauroyl alanine and sodium methyl cocoyl taurate were stronger than that of AES.展开更多
The precipitate and the coacervate are two aggregated states in the polyelectrolyte complexes(PECs).The precipitate-to-coacervate transition and glass transition in PECs have been widely reported in the past.In many c...The precipitate and the coacervate are two aggregated states in the polyelectrolyte complexes(PECs).The precipitate-to-coacervate transition and glass transition in PECs have been widely reported in the past.In many cases,the two phenomena are studied independently,although both of them are apparently affected by water and small ions.Here,utilizing a PEC system consisting of poly(acrylic acid)(PAA)and a cationic bolaamphiphile(DBON),we explore the states of PECs as a function of salt,temperature,and the molecular weight of PAAs.By a combination of microscopic observation,time-resolved fluorescence measurements,and differential scanning calorimetry,we identify salt/temperature driven precipitate-to-coacervate transitions of the complexes.The thermally induced morphology transformation from the precipitate to coacervate occurs around the glass transition temperature,indicating a strong correlation between the two processes.As the molecular weight of the PAA increases,the thermal transition temperature becomes higher.This finding offers new insights on the mechanistic interactions that dictate the aggregated states of PECs.Based on the photothermal effect of DBON,we also develop a UV light-induced strategy to mediate the precipitate-to-coacervate transition,providing a fantastic platform to create functional PEC materials.展开更多
Coacervation of oxidized glutathione(GSSG)and a cationic surfactant,didodecyldimethylammonium bromide(DDAB),was constructed mainly driven by the electrostatic and hydrophobic interactions.The pH-dependent coacervate o...Coacervation of oxidized glutathione(GSSG)and a cationic surfactant,didodecyldimethylammonium bromide(DDAB),was constructed mainly driven by the electrostatic and hydrophobic interactions.The pH-dependent coacervate of GSSG-DDAB(1∶4,mol/mol)was analyzed.Under acidic and neutral conditions,a turbid suspension of droplets is observed,and alkaline pH results in the phase separation of coacervates as the top phase.The coacervate phase exhibits good performance(extraction efficiency>85%)in extracting several dyes from water,including brilliant yellow,acid red 13,cresyl violet acetate,eriochrom blue SE,and 4-hydroxyazobenzene.The dyes are added into the suspension in acidic conditions.Then,the dyes are enriched and extracted along with the coacervates as the top phase when pH is adjusted to~10.Coacervation of GSSG with DDAB provides a simple approach to extract organic pollutants in wastewater treatment.展开更多
Distribution of TX114 between coacervate and aqueous phases in clouding of various initial TX114 concentrations was studied. Effects of temperature and salinity （Na2SO4） on the distribution of TX114 concentration we...Distribution of TX114 between coacervate and aqueous phases in clouding of various initial TX114 concentrations was studied. Effects of temperature and salinity （Na2SO4） on the distribution of TX114 concentration were also investigated. Differing from the nonionic surfactant C12E10, the distribution of TX114 is sensitive to the temperature, and it is observed that the TX114 concentration in the aqueous phase （Caq） does not depend on the initial TX114 concentration apparently at 45℃, and the Caq decreases with an increase of NazSO4 concentration. Low initial TX114 concentration in unclouded solutions, high Na2SO4 concentration, and temperature are suggested to control the surfactant loss in large-scale cloud point extraction applications.展开更多
Adhesives have attracted a great deal of attention as an advanced modality in biomedical engineering because of their unique wound management behavior.However,it is a grand challenge for current adhesive systems to ac...Adhesives have attracted a great deal of attention as an advanced modality in biomedical engineering because of their unique wound management behavior.However,it is a grand challenge for current adhesive systems to achieve robust adhesion due to their tenuous interfacial bonding strength.Moreover,the absence of dynamic adaptability in conventional chemical adhesives restricts neoblasts around the wound from migrating to the site,resulting in an inferior tissue-regeneration effect.Herein,an extracellular matrix-derived biocomposite adhesive with robust adhesion and a real-time skin healing effect is well-engineered.Liquid–liquid phase separation is well-harnessed to drive the assembly of the biocomposite adhesive,with the active involvement of supramolecular interactions between chimeric protein and natural DNA,leading to a robustly reinforced adhesion performance.The bioadhesive exhibits outstanding adhesion and sealing behaviors,with a sheared adhesion strength of approximately 18 MPa,outperforming its reported counterparts.Moreover,the engineered bioderived components endow this adhesive material with biocompatibility and exceptional biological functions including the promotion of cell proliferation and migration,such that the use of this material eventually yields real-time in situ skin regeneration.This work opens up novel avenues for functionalized bioadhesive engineering and biomedical translations.展开更多
基金supported by the National Key Research and Development Program of China(Nos.2023YFD1900602 and 2023YFD1900605)the Fundamental Research Funds for the Central Universities(No.SWU-KR24036)the Visiting Training Funds for Teachers from Ordinary Undergraduate Colleges and Universities in Shandong Province.
文摘Phosphorus(P)is crucial for crop growth.However,in waters,P is considered as contaminant due to its role in causing eutrophication and algae blooms.Therefore,recovering P from wastewater is essential for sustainable P management.This study investigated the removal of P from aqueous solutions using bioinspired poly(ethylenimine)-poly(acrylamideco-acrylic acid)(PEI-PAMcoAA)coacervates.In detail,we investigated various parameters affecting P removal,including the ratio of PEI to PAMcoAA(ranging from 1:2 to 3:1,stoichiometry ratio of NH_(2) to COOH),pH(5.0-8.0)of P-containing solutions,initial P concentration(0.05-5 mmol/L),and the addition of calcium(Ca,0.1-5 mmol/L).We found that increasing the PEI:PAMcoAA ratio from1:2 to 3:1 significantly enhanced P removal efficiency,increasing from 47.21%to 95.44%.Under neutral pH conditions without calcium(Ca),PEI-PAMcoAA coacervates demonstrated optimal P removal capabilities(achieving an efficiency of 77.96%)through electrostatic adsorption.In contrast,the addition of Ca under alkaline conditions markedly improved P removal efficiency,increasing it from 64.16%to 82.42%.Detailed analyses of P within the coacervates indicated that Ca facilitates P precipitation and provides additional binding sites.These findings demonstrated that PEI-(Ca)-PAMcoAA coacervates show promise for efficiently removing P,particularly at low P concentrations.After the Premoval,the immobilized P can potentially be reused directly,as P able to be released from the reacted products.Therefore,the reacted coacervates could serve as a non-toxic fertilizer.Given its simplicity,high efficiency,and environmental friendliness,P removal based on bioinspired coacervates represents a low-hanging fruit in the pursuit of sustainable P management.
基金supported by the National Natural Science Foundation of China(No.21973002).
文摘The liquid-liquid phase separation of biopolymers in living cells contains multiple interactions and occurs in a dynamic environment.Resolving the regulation mechanism is still a challenge.In this work,we designed a series of peptides(XXLY)_(6)SSSGSS and studied their complexation and coacervation behavior with single-stranded oligonucleotides.The“X”and“Y”are varied to combine known amounts of charged and non-charged amino acids,together with the introduction of secondary structures and pH responsiveness.Results show that the electrostatic interaction,which is described as charge density,controls both the strength of complexation and the degree of chain relaxation,and thus determines the growth and size of the coacervates.The hydrophobic interaction is prominent when the charges are neutralized.Interestingly,the secondary structures of peptides exhibit profound effect on the morphology of the phases,such as solid phase to liquid phase transition.Our study gains insight into the phase separation under physiological conditions.It is also helpful to create coacervates with desirable structures and functions.
基金financially supported by the National Key R&D Program of China(No.2022YFB3805103)the National Natural Science Foundation of China(No.22178139)。
文摘Significant progress has been made in wet adhesives for low salinity water,but exploration of general ionic adhesives for natural seawater is less developed because the high salinity could weaken interfacial bonding and shields electrostatic interactions,resulting in adhesion failure.Thus,the design of adhesives for natural seawater represents challenges less resolved.Herein,a cationic polyelectrolyte(PECHIA)containing imidazolacetonitrile unit was explored to prepare adhesives enabled by natural seawater.By combining the ion shielding effect with the“cation-dipole”interactions between PECHIA chains,aqueous solution of the PECHIA underwent coacervation and self-crosslinking in natural seawater,allowing for underwater adhesion to various substrates in seawater.The instantaneous lap-shear and tensile adhesion strengths are 47 and 119 kPa,respectively,while the cured adhesive shows~739 k Pa tensile adhesion in natural seawater.The design of PECHIA enables wet adhesives viable for applications in the diversified scenarios of natural seawater.
基金the National Natural Science Foundation of China(Grant no.81373045)the Provincial Natural Science Foundation of Hubei of China(Grant no.2015CFA139)
文摘Hexafluoroisopropanol(HFIP)-induced sodium dodecyl sulfate/dodecyltrimethylammonium bromide(SDS/DTAB) catanionic surfactant coacervate extraction method coupled with high performance liquid chromatography(HPLC) was used to detect the migration of phthalates from disposable tablewares to drinking water. The concentration factors are larger than 82 and extraction recoveries over 53% for water samples spiked with 100 or 200 ng/m L phthalates. Limit of detection is in the range of 1.0–2.6 ng/m L.Good linearity with correlation coefficients larger than 0.9985 is obtained in the concentration of20–1500 or 40–3000 ng/m L. Relative recoveries are from 82.4% to 123.6% for water samples spiked with30/60, 250/500, and 1500/3000 ng/m L phthalates, respectively. Relative standard deviations(RSDs) are0.4%–7.4% for intraday precision(n = 5) and 0.6%–7.8% for interday precision(n = 3). Four of studied phthalates are found in the drinking water samples prepared from four kinds of tablewares.
文摘The microstructure of CdI2 thin film grown during vapor-phase deposition was investigated by scanning electron microscopy (SEM). The thin film deposited on Si crystal consists of numerous sunflower-like aggregates. These aggregates display well self-assembly characteristics. The size of Sunflower-like aggregates is between 12 and 44 μm. Each sunflower-like aggregate is surrounded with many adjacent wings-'petals'. The structure of central region of the 'sunflower' is obviously difFerent from that of the 'petal'. Electron spectroscopy for chemical analysis (ESCA) was employed in determining the chemical valence of the thin film. Self-organization efFect is used to explain the coring growth process of CdI2 thin film
基金supported by the National Nature Science Foundation of China(No.82073286)State Key Laboratory of Neurology and Oncology Drug Development(No.SKLSIM-F202418,China).
文摘Liquid–liquid phase separation(LLPS)induces the formation of membrane-less droplet-like compartments through the segregation of biomolecules into distinct liquid phases within a solution,without the requirement for a surrounding lipid bilayer1.These membrane-less droplet-like compartments,which arise from LLPS,possess unique properties and functions essential for cellular organization,biomolecular condensation,and cellular signaling2.
基金supported by the National Key Research and Development Project,China(No.2020YFA0909000)the National Natural Science Foundation of China(No.22107027)+4 种基金the Science and Technology Innovation Program of Hunan Province(No.2024RC3099)the Natural Science Foundation of Hunan Province,China(No.2023JJ20003)the Scientific Research Program of Furong Laboratory,China(No.2023SK2088)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515220118)the Hunan Provincial Innovation Foundation for Postgraduate,China(No.CX20230409).
文摘Recent progress in nanotechnology and synthetic biology has demonstrated the potential of DNA coacervates for biomimetic and biological applications.DNA coacervates are micron-scale,membrane-free,spherical structures formed by liquid-liquid phase separation of DNA materials.They uniquely combine the programmability of DNA with the fluidic properties of coacervates,allowing for controlled modulation of their structures,biomimetic and biological functions,and dynamic behaviors through rational sequence design.This review summarizes methods for the formation of different DNA coacervates and explores their extensive applications in biomimicry,biosensing and therapeutics.Limitations and prospects of DNA coacervates are also discussed.
文摘Controlled delivery of proteins and other biologics is a growing medium of therapy for diseases previously untreatable.Here we report a self-assembling,tunable vesicle for the controlled delivery of growth factors and cytokines.Coacervate made of heparin and a biocompatible polycation,PEAD,forms the core of the vesicle;lipids form the membrane of the vesicle.We call this vesicle lipocoacervate(LipCo),which has a high affinity for growth factors and cytokines due to heparin.LipCo is a tunable protein delivery vehicle.The vesicle size is controlled through polymer and salt concentrations.Membrane functionalization enables potential for targeting capabilities with long-term storage through lyophilization.Importantly,the controlled delivery of therapeutics also avoids high toxicity to treated cells in vitro.Here we report on these key principles of LipCo assembly and design.
基金Chongqing Postdoctoral International Exchange Training Program(7820100997)Fundamental Research Funds for Central Universities(Nos.SWU-XDPY22010)+2 种基金National College Students Innovation and Entrepreneurship Training Program(202310635114)National Natural Science Foundation of China(No.81703424)Chongqing Graduate Student Research Innovation Project(CYB21121).
文摘Developing an oral in situ-forming hydrogel that targets the inflamed intestine to suppress bleeding ulcers and alleviate intestinal inflammation is crucial for effectively treating ulcerative colitis(UC).Here,inspired by sandcastle worm adhesives,we proposed a water-immiscible coacervate(EMNs-gel)with a programmed coacervate-to-hydrogel transition at inflammatory sites composed of dopa-rich silk fibroin matrix containing embedded inflammation-responsive core-shell nanoparticles.Driven by intestinal peristalsis,the EMNs-gel can be actuated forward and immediately transform into a hydrogel once contacting with the inflamed intestine to yield strong tissue adhesion,resulting from matrix metalloproteinases(MMPs)-triggered release of Fe3+from embedded nanoparticles and rearrangement of polymer network of EMNs-gel on inflamed intestine surfaces.Extensive in vitro experiments and in vivo UC models confirmed the preferential hydrogelation behavior of EMNs-gel to inflamed intestine surfaces,achieving highly effective hemostasis,and displaying an extended residence time(48 h).This innovative EMNs-gel provides a non-invasive solution that accurately suppresses severe bleeding and improves intestinal homeostasis in UC,showcasing great potential for clinical applications.
基金the projects of National Natural Science Foundation of China(No.32301209)Key R&D Projects of Henan Province(Nos.231111312400 and 241111220400).
文摘Engineering hydrogels that resemble biological tissues of various lengths via conventional fabrication techniques remains challenging.Three-dimensional(3D)bioprinting has emerged as an advanced approach for constructing complex biomimetic 3D architectures,which are currently restricted by the limited number of available bioinks with high printability,biomimicry,biocompatibility,and proper mechanical properties.Inspired by ubiquitous coacervation phenomena in biology,we present a unique mineral-biopolymer coacervation strategy that enables the hierarchical assembly of nanoclay and recombinant human collagen(RHC).This system was observed to undergo a coacervation transition(liquid‒liquid phase separation)spontaneously.The formed dense phase separated from its supernatant is the coacervate of clay-RHC-rich complexes,where polymer chains are sandwiched between silicate layers.Molecular dynamics simulation was first used to verify and explore the coacervation process.Then,the coacervates were demonstrated to be potential bioinks that exhibited excellent self-supporting and shear-thinning viscoelastic properties.Through extrusion-based printing,the versatility of the bioink was demonstrated by reconstructing the key features of several biological tissues,including multilayered lattice,vascular,nose,and ear-like structures,without the need for precrosslinking operations or support baths.Furthermore,the printed scaffolds were cytocompatible,elicited minimal inflammatory responses,and promoted bone regeneration in calvarial defects.
基金supported by the National Natural Science Foundation(No.32271468)Sichuan Science and Technology Program(No.2021JDTD0001)+2 种基金1·3·5 Project for disciplines of excellence,West China Hospital,Sichuan University(No.ZYYC23005)the Fundamental Research Funds for the Central Universities(No.2022SCU12046)Innovation Research Project of Sichuan University(No.2022SCUH0046).
文摘Oral ulcers are a common ulcerative injury that occurs in the oral mucosa.When occurring,they can cause mucosal pain and affect eating and communication.The oral cavity,characterized by its moist environment and constant movement of the lips and tongue,presents challenges for conventional drug delivery systems due to its suboptimal adhesion.Therefore,there is a need for the development of adhesive materials specifically designed for use within the oral cavity.In this research,a sticky coacervate incorporating tea polyphenols(TP)was formulated based on the adhesive properties observed in sandcastle worms.The coacervate is composed of Pluronic F68(F68)and TP,synthesized through the coacervation reaction.The F68-TP coacervates are attached to porcine skin easily.It also reduces bacterial viability and has the ability to clear reactive oxygen species.In animal ulcer models,these coacervates demonstrate anti-inflammatory effects and enhance collagen and muscle fiber synthesis.Overall,these adhesive coacervates with antioxidative and antibacterial properties hold potential as a therapeutic option for oral ulcers in the oral cavity.
基金This work was supported by grants from Advanced Postdoctoral Programs of Zhejiang(zj2019030)China Postdoctoral Science Foundation(2019M662015)+1 种基金Research Unit of Research and Clinical Translation of Cell Growth Factors and Diseases,Chinese Academy of Medical Science(No.2019RU010 to X.L.)CAMS Innovation Fund for Medical Sciences(2019-I2M-5-028),China.
文摘Heart disease is still the leading killer all around the world,and its incidence is expected to increase over the next decade.Previous reports have already shown the role of fibroblast growth factor10(FGF10)in alleviating heart diseases.However,FGF10 has not been used to treat heart diseases because the free protein has short half-life and low bioactivity.Here,an injectable coacervate was designed to protect growth factor from degradation during delivery and the effects of the FGF10 coacervate were studied using a mice acute myocardial infarction(MI)model.As shown in our echocardiographic results,a single injection of FGF10 coacervate effectively inhibited preserved cardiac contractibility and ventricular dilation when compared with free FGF10 and the saline treatment 6 weeks after MI.It is revealed in histological results that the MI induced myocardial inflammation and fibrosis was reduced after FGF10 coacervate treatment.Furthermore,FGF10 coacervate treatment could improve arterioles and capillaries stabilization through increasing the proliferation of endothelial and mural cells.However,with the same dosage,no statistically significant difference was shown between free FGF10,heparin+FGF10 and saline treatment,especially in long term.On another hand,FGF10 coacervate also increased the expression of cardiac-associated the mRNA(cTnT,Cx43 and α-SMA),angiogenic factors(Ang-1 and VEGFA)and decreased the level of inflammatory factor(tumor necrosis factor-α).The downstream signaling of the FGF10 was also investigated,with the western blot results showing that FGF10 coacervate activated the p-FGFR,PI3K/Akt and ERK1/2 pathways to a more proper level than free FGF10 or heparin+FGF10.In general,it is revealed in this research that one-time injection of FGF10 coacervate sufficiently attenuated MI induced injury when compared with an equal dose of free FGF10 or heparin+FGF10 injection.
基金the National Key Research and Development Program(2022YFB3804403)the Collaborative Research Fund from the Research Grants Council of Hong Kong(Project No.C5044-21G)+1 种基金the Research Grants Council of the Hong Kong Special Administration Region(project no.GRF/14202920,GRF/14204618,GRF/14108720,T13-402/17-N and AoE/M-402/20)National Natural Science Foundation of China(22205264).
文摘Protecting the skin from UV light irradiation in wet and underwater environments is challenging due to the weak adhesion of existing sunscreen materials but highly desired.Herein we report a polyethyleneimine/thioctic acid/titanium dioxide(PEI/TA/TiO_(2))coacervate-derived hydrogel with robust,asymmetric,and reversible wet bioadhesion and effective UV-light-shielding ability.The PEI/TA/TiO_(2)complex coacervate can be easily obtained by mixing a PEI solution and TA/TiO_(2)powder.The fluid PEI/TA/TiO_(2)coacervate deposited on wet skin can spread into surface irregularities and subsequently transform into a hydrogel with increased cohesion,thereby establishing interdigitated contact and adhesion between the bottom surface and skin.Meanwhile,the functional groups between the skin and hydrogel can form physical interactions to further enhance bioadhesion,whereas the limited movement of amine and carboxyl groups on the top hydrogel surface leads to low adhesion.Therefore,the coacervate-derived hydrogel exhibits asymmetric adhesiveness on the bottom and top surfaces.Moreover,the PEI/TA/TiO_(2)hydrogel formed on the skin could be easily removed using a NaHCO3 aqueous solution without inflicting damage.More importantly,the PEI/TA/TiO_(2)hydrogel can function as an effective sunscreen to block UV light and prevent UV-induced MMP-9 overexpression,inflammation,and DNA damage in animal skin.The advantages of PEI/TA/TiO_(2)coacervate-derived hydrogels include robust,asymmetric,and reversible wet bioadhesion,effective UV light-shielding ability,excellent biocompatibility,and easy preparation and usage,making them a promising bioadhesive to protect the skin from UV light-associated damage in wet and underwater environments.
基金supported by National Natural Science Foundation of China(grant nos.21972149,21988102,21811530002,21633002,and 21761142007).
文摘Low-molecular weight surfactants have significant potential as building blocks for prebiotic organization.However,reports about surfactant-based coacervates as protocell models capable of reversible transformation are scarce.Herein,we develop a simple system made of a surfactant(-)-N-dodecylN-methylephedrinium bromide(DMEB)and inorganic salts that is capable of spontaneous formation of vesicles,coacervates,and the reversible transformation between the two states.
基金Singapore National Research Fellowship,Grant/Award Number:NRF-NRFF11-2019-0004Singapore Ministry of Education,Grant/Award Number:MOE-T2EP30220-0006。
文摘Many functional coacervates have been identified in biological systems,which have attracted widespread interest.Coacervation is a liquid–liquid phase separation(LLPS)process in which a macromolecule-enriched liquid phase is formed together with a macromolecule-depleted phase.Bio-inspired coacervates possess excellent features such as underwater delivery,low interface energy,shear thinning,and excellent biocompatibility.They also serve as good delivery platforms for different types of molecules.In this review,we briefly discuss some important extracellular coacervate systems,including mussel adhesives,sandcastle worm glue,squid beak,and tropoelastin.We then provide an overview of the recent development of bio-inspired functional coacervates for various biomedical applications,including medical adhesives,drug delivery,and tissue engineering.Bio-inspired functional coacervates offer a promising material platform for developing new materials for biomedical applications.
文摘Using sodium laureth sulfate(AES)as reference,the effects of different pH values on the foam properties of four amino acid surfactants(sodium lauroyl sarcosinate,lauroyl alanine,disodium cocoyl glutamate,sodium methyl cocoyl taurate)were compared.On the basis,the effects of amino acid surfactants on foam performance,flocculation behavior,hair color protection efficacy and sebum removal capacity were studied when AES was completely or partially replaced by amino acid surfactant,and the correlation between the structure of amino acid surfactant and these properties was discussed.Compared with AES,the foam performance of sodium lauroyl sarcosinate,lauroyl alanine and disodium cocoyl glutamate were significantly affected by pH value,and sodium methyl cocoyl taurate was less affected.The foam stability of shampoo system can be enhanced by the combination of amino acid surfactant,and the foam performance of shampoo system can be significantly improved by the combination of sodium methyl cocoyl taurate.All the four amino acid surfactants can prolong the flocculation time of shampoo,and the effect of disodium cocoyl glutamate was the most obvious.The hair color protection efficacy of disodium cocoyl glutamate and sodium methyl cocoyl taurate were better than AES.The degreasing power of disodium cocoyl glutamate was weaker than that of AES,and the degreasing power of sodium lauroyl sarcosinate,lauroyl alanine and sodium methyl cocoyl taurate were stronger than that of AES.
基金State Key Research Development Programme of China,Grant/Award Number:2021YFB3800702National Natural Science Foundation of China,Grant/Award Number:21902073+1 种基金Shenzhen Science and Technology Innovation Committee,Grant/Award Number:JSGG20210629144802007Post-Doctoral Later-Stage Foundation Project of Shenzhen Polytechnic,Grant/Award Number:6021271003K。
文摘The precipitate and the coacervate are two aggregated states in the polyelectrolyte complexes(PECs).The precipitate-to-coacervate transition and glass transition in PECs have been widely reported in the past.In many cases,the two phenomena are studied independently,although both of them are apparently affected by water and small ions.Here,utilizing a PEC system consisting of poly(acrylic acid)(PAA)and a cationic bolaamphiphile(DBON),we explore the states of PECs as a function of salt,temperature,and the molecular weight of PAAs.By a combination of microscopic observation,time-resolved fluorescence measurements,and differential scanning calorimetry,we identify salt/temperature driven precipitate-to-coacervate transitions of the complexes.The thermally induced morphology transformation from the precipitate to coacervate occurs around the glass transition temperature,indicating a strong correlation between the two processes.As the molecular weight of the PAA increases,the thermal transition temperature becomes higher.This finding offers new insights on the mechanistic interactions that dictate the aggregated states of PECs.Based on the photothermal effect of DBON,we also develop a UV light-induced strategy to mediate the precipitate-to-coacervate transition,providing a fantastic platform to create functional PEC materials.
文摘Coacervation of oxidized glutathione(GSSG)and a cationic surfactant,didodecyldimethylammonium bromide(DDAB),was constructed mainly driven by the electrostatic and hydrophobic interactions.The pH-dependent coacervate of GSSG-DDAB(1∶4,mol/mol)was analyzed.Under acidic and neutral conditions,a turbid suspension of droplets is observed,and alkaline pH results in the phase separation of coacervates as the top phase.The coacervate phase exhibits good performance(extraction efficiency>85%)in extracting several dyes from water,including brilliant yellow,acid red 13,cresyl violet acetate,eriochrom blue SE,and 4-hydroxyazobenzene.The dyes are added into the suspension in acidic conditions.Then,the dyes are enriched and extracted along with the coacervates as the top phase when pH is adjusted to~10.Coacervation of GSSG with DDAB provides a simple approach to extract organic pollutants in wastewater treatment.
基金Supported by the National Natural Science Foundation of China （20676069）.
文摘Distribution of TX114 between coacervate and aqueous phases in clouding of various initial TX114 concentrations was studied. Effects of temperature and salinity （Na2SO4） on the distribution of TX114 concentration were also investigated. Differing from the nonionic surfactant C12E10, the distribution of TX114 is sensitive to the temperature, and it is observed that the TX114 concentration in the aqueous phase （Caq） does not depend on the initial TX114 concentration apparently at 45℃, and the Caq decreases with an increase of NazSO4 concentration. Low initial TX114 concentration in unclouded solutions, high Na2SO4 concentration, and temperature are suggested to control the surfactant loss in large-scale cloud point extraction applications.
基金supported by the National Key Research and Development Program of China(2022YFA0913200 and 2021YFB3502300)the National Natural Science Foundation of China(22020102003,22125701,22277064,82272161,52222214,and 22107097)+3 种基金Beijing Municipal Science and Technology Commission(221100007422088)Beijing Nova Program(Z211100002121132)Beijing Natural Science Foundation(2222010)Xiangfu Lab Research Project(XF012022C0200)。
文摘Adhesives have attracted a great deal of attention as an advanced modality in biomedical engineering because of their unique wound management behavior.However,it is a grand challenge for current adhesive systems to achieve robust adhesion due to their tenuous interfacial bonding strength.Moreover,the absence of dynamic adaptability in conventional chemical adhesives restricts neoblasts around the wound from migrating to the site,resulting in an inferior tissue-regeneration effect.Herein,an extracellular matrix-derived biocomposite adhesive with robust adhesion and a real-time skin healing effect is well-engineered.Liquid–liquid phase separation is well-harnessed to drive the assembly of the biocomposite adhesive,with the active involvement of supramolecular interactions between chimeric protein and natural DNA,leading to a robustly reinforced adhesion performance.The bioadhesive exhibits outstanding adhesion and sealing behaviors,with a sheared adhesion strength of approximately 18 MPa,outperforming its reported counterparts.Moreover,the engineered bioderived components endow this adhesive material with biocompatibility and exceptional biological functions including the promotion of cell proliferation and migration,such that the use of this material eventually yields real-time in situ skin regeneration.This work opens up novel avenues for functionalized bioadhesive engineering and biomedical translations.
