Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review ...Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.展开更多
The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with th...The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.展开更多
The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium...The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium alginate-based multilayer film is fabricated via a layer-by-layer(LBL)self-assembly method.With the help of superior interaction between the layers,the multilayer film possesses excellent mechanical properties(with a tensile strength of 50 MPa).Besides,the film displays outstanding water retention property(blocking moisture of 97.56%)and ultraviolet blocking property.Anthocyanin is introduced into the film to detect the food quality since it is one natural plant polyphenol that is sensitive to the pH changes ranging from 1 to 13 in food when spoilage occurs.It is noted that the film is also bacteriostatic which is desired for food packaging.This study describes a simple technique for the development of advanced multifunctional and fully biodegradable food packaging film and it is a sustainable alternative to plastic packaging.展开更多
Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their mac...Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.展开更多
We consider the inverse problem of finding guiding pattern shapes that result in desired self-assembly morphologies of block copolymer melts.Specifically,we model polymer selfassembly using the self-consistent field t...We consider the inverse problem of finding guiding pattern shapes that result in desired self-assembly morphologies of block copolymer melts.Specifically,we model polymer selfassembly using the self-consistent field theory and derive,in a non-parametric setting,the sensitivity of the dissimilarity between the desired and the actual morphologies to arbitrary perturbations in the guiding pattern shape.The sensitivity is then used for the optimization of the confining pattern shapes such that the dissimilarity between the desired and the actual morphologies is minimized.The efficiency and robustness of the proposed gradient-based algorithm are demonstrated in a number of examples related to templating vertical interconnect accesses(VIA).展开更多
Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we ut...Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we utilized the phosphorylation sites of collagen molecules to combine with cobalt-based mononuclear precursors at the molecular level and built a three-dimensional(3D)porous hierarchical material through a bottom-up biomimetic self-assembly strategy to obtain single-atom catalysts confined on carbonized biomimetic self-assembled carriers(Co SACs/cBSC)after subsequent high-temperature annealing.In this strategy,the biomolecule improved the anchoring efficiency of the metal precursor through precise functional groups;meanwhile,the binding-then-assembling strategy also effectively suppressed the nonspecific adsorption of metal ions,ultimately preventing atomic agglomeration and achieving strong electronic metal-support interactions(EMSIs).Experimental characterizations confirm that binding forms between cobalt metal and carbonized self-assembled substrate(Co–O_(4)–P).Theoretical calculations disclose that the local environment changes significantly tailored the Co d-band center,and optimized the binding energy of oxygenated intermediates and the energy barrier of oxygen release.As a result,the obtained Co SACs/cBSC catalyst can achieve remarkable OER activity and 24 h durability in 1 M KOH(η10 at 288 mV;Tafel slope of 44 mV dec-1),better than other transition metal-based catalysts and commercial IrO_(2).Overall,we presented a self-assembly strategy to prepare transition metal SACs with strong EMSIs,providing a new avenue for the preparation of efficient catalysts with fine atomic structures.展开更多
Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface mo...Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface morphology and electric property was investigated.The results confirmed the dense membrane of PEDOT:PSS and the lamellar structure of PDDA-rGO on the fibers.It has excellent electrical conductivity and mechanical properties.The fiber based electrochemical transistor(FECTs)prepared by the composite conductive fiber has a maximum output current of 8.7 mA,a transconductance peak of 10 mS,an on time of 1.37 s,an off time of 1.6 s and excellent switching stability.Most importantly,the devices by layer by layer self-assembly technology opens a path for the true integration of organic electronics with traditional textile technologies and materials,laying the foundation for their later widespread application.展开更多
New concept for the development of supramolecular assemblies from intricate inter-actions between different classes of biomacromolecules(polysaccharides,proteins and lipids)is yet to come,due to their intrinsic chemic...New concept for the development of supramolecular assemblies from intricate inter-actions between different classes of biomacromolecules(polysaccharides,proteins and lipids)is yet to come,due to their intrinsic chemical and structural complex-ity and incompatibility.Herein,we report an interaction mechanism among multiple biomacromolecules,and the structural and digestive properties of their assemblies using amylose(AM),lauric acid(LA),andβ-lactoglobulin(βLG)as exemplars.AM,LA,andβLG interact to form a water-soluble ternary complex through van der Waals forces between AM and LA and high affinity binding between AM andβLG,which can further assemble into uniform-sized,semi-crystalline nanospheres under certain thermodynamic conditions.These nanospheres are substantially resis-tant to amylolysis,thus can be well utilized by gut microbiota,including increasing short-chain fatty acid levels and shaping bacterial communities.Illustrating the com-plexation of AM,LA,andβLG and their assemblies from disorder to order,this work offers potential rationale of assemblies for multiple biomacromolecules driven by non-covalent interactions and substantial potentials for supramolecular biomaterials development.展开更多
Ferroptosis has emerged as a potent form of no-apoptotic cell death that offers a promising alternative to avoid the chemoresistance of apoptotic pathways and serves as a vulnerability of cancer.Herein,we have constru...Ferroptosis has emerged as a potent form of no-apoptotic cell death that offers a promising alternative to avoid the chemoresistance of apoptotic pathways and serves as a vulnerability of cancer.Herein,we have constructed a biomimetic self-assembly nano-prodrug system that enables the co-delivery of gefitinib(Gefi),ferrocene(Fc)and dihydroartemisinin(DHA)for the combined therapy of both ferroptosis and apoptosis.In the tumor microenvironment,this nano-prodrug is able to disassemble and trigger drug release under high levels of GSH.Interestingly,the released DHA can downregulate GPX4 level for the enhancement of intracellular ferroptosis from Fc,further executing tumor cell death with concomitant chemotherapy by Gefi.More importantly,this nano-prodrug provides highly homologous targeting ability by coating related cell membranes and exhibits outstanding inhibition of tumor growth and metastasis,as well as no noticeable side-effects during treatments.This simple small molecular self-assembled nano-prodrug provides a new reasonably designed modality for ferroptosis-combined chemotherapy.展开更多
Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;howe...Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;however,the improvement of their energy density remains a challenge.Here,we design a green and universal approach to prepare the composite electrode material,which is composed of lignin-phenolformaldehyde resins derived hierarchical porous carbon(LR-HPC)as conductive skeletons and the self-assembly manganese cobaltite(MnCo_(2)O_(4))nanocrystals as active sites.The synthesized C@MnCo_(2)O_(4)composite has an abundant porous structure and superior electronic conductivity,allowing for more charge/electron mass transfer channels and active sites for the redox reactions.The composite shows excellent electrochemical performance,such as the maximum specific capacitance of~726 mF cm^(-2)at 0.5 mV s^(-1),due to the significantly enhanced interactive interface between LR-HPC and MnCo_(2)O_(4)crystals.The assembled all-solid-state asymmetric supercapacitor,with the LR-HPC and C@MnCo_(2)O_(4)as cathode and anode,respectively,exhibits the highest volumetric energy density of 0.68 mWh cm^(-3)at a power density of 8.2 mW cm^(-3).Moreover,this device shows a high capacity retention ratio of~87.6%at 5 mA cm^(-2)after 5000 cycles.展开更多
NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy leve...NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.展开更多
Traditional Chinese medicine decoction is a complex polydispersed phase system containing real solution,colloid solution,emulsion and suspension.The compound decoction of traditional Chinese medicine has complex compo...Traditional Chinese medicine decoction is a complex polydispersed phase system containing real solution,colloid solution,emulsion and suspension.The compound decoction of traditional Chinese medicine has complex components,including saponins,alkaloids,polysaccharides,flavonoids,amino acids and so on,which can be self-assembled to form gels,fibers,micelles,vesicles and so on.The self-assembled nano-phase not only neutralizes the single drug and reduces the toxicity and side effects,but also has its own pharmacological effects,which complement each other to achieve synergistic effect,so as to achieve the role of drug supplement,which is of research significance.The formation principle,solubilization and synergism principle and characterization method of multi-component self-assembly of traditional Chinese medicine compound decoction are discussed in this paper.展开更多
Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance ...Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance as the thickness increases,caused by increasing ion diffusion limitation.Further limitations include restacking of the nanosheets,which makes it challenging to realize the full potential of these electrode materials.Herein,we demonstrate the design of a vertically aligned MXene hydrogel composite,achieved by thermal-assisted self-assembled gelation,for high-rate energy storage.The highly interconnected MXene network in the hydrogel architecture provides very good electron transport properties,and its vertical ion channel structure facilitates rapid ion transport.The resulting hydrogel electrode show excellent performance in both aqueous and organic electrolytes with respect to high capacitance,stability,and high-rate capability for up to 300μm thick electrodes,which represents a significant step toward practical applications.展开更多
Myocardial infarction accompanied by diabetes mellitus is accepted as the most seri-ous type of coronary heart disease,and among the current treatment strategies,the precise delivery of protective drugs for inhibiting...Myocardial infarction accompanied by diabetes mellitus is accepted as the most seri-ous type of coronary heart disease,and among the current treatment strategies,the precise delivery of protective drugs for inhibiting cardiomyocyte apoptosis is still a challenge.In this study,we developed a biodegradable nanoparticles-based delivery system with excellent macrophage escape,cardiac targeting,and drug release prop-erties to achieve targeted therapy of myocardial infarction.Specifically,a copolymer of p(DMA–MPC–CD)combining self-adhesion,hydration lubrication,and targeting peptide binding site was successfully prepared by free radical copolymerization,and it was self-assembled on the surface of melatonin-loaded dendritic mesoporous silica nanoparticles(bMSNs)following the integration of adamantane-modified cardiac homing peptide(CHP)based on supramolecular host–guest interaction.Importantly,a hydration layer formed around the zwitterionic phosphorylcholine groups of the multifunctional nanoparticles,which was confirmed by the enhancement in hydra-tion lubrication and reduction in coefficient of friction,prevented the nanoparticles from phagocytosis by the macrophages.The in vivo bioluminescence imaging test indicated that the nanoparticles were endowed with satisfied cardiac targeting capa-bility,and the in vivo mice study demonstrated that the intravenous injection of drug-loaded nanoparticles(namely bMSNs–Mel@PDMC–CHP)effectively reduced cardiomyocyte apoptosis,alleviated myocardial interstitialfibrosis,and enhanced cardiac function.展开更多
Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited b...Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.展开更多
The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate str...The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate strategies for designing anti-fouling surfaces are crucial.Here,we employ molecular dynamics simulations and alchemical free energy calculations to systematically analyze the factors influencing resistance to protein adsorption on the SAMs terminated with single or double OH groups at three packing densities(∑=2.0 nm^(-2),4.5 nm^(-2),and 6.5 nm^(-2)),respectively.For the first time,we observed that the compactness and order of interfacial water enhance its physical barrier effect,subsequently enhancing the resistance of SAM to protein adsorption.Notably,the spatial hindrance effect of SAM leads to the embedding of protein into SAM,resulting in a lack of resistance of SAM towards protein.Furthermore,the number of hydroxyl groups per unit area of double OH-terminated SAM at ∑=6.5 nm^(-2) is approximately 2 to 3 times that of single OH-terminated SAM at ∑=6.5 nm^(-2) and 4.5 nm^(-2),consequently yielding a weaker resistance of double OH-terminated SAM towards protein.Meanwhile,due to the structure of SAM itself,i.e.,the formation of a nearly perfect ice-like hydrogen bond structure,the SAM exhibits the weakest resistance towards protein.This study will complement and improve the mechanism of OH-SAM resistance to protein adsorption,especially the traditional barrier effect of interfacial water.展开更多
Bio-based cyclodextrins(CDs)are a common research object in supramolecular chemistry.The special cavity structure of CDs can form supramolecular self-assemblies such as vesicles and microcrystals through weak interact...Bio-based cyclodextrins(CDs)are a common research object in supramolecular chemistry.The special cavity structure of CDs can form supramolecular self-assemblies such as vesicles and microcrystals through weak interaction with guest molecules.The different forms of supramolecular self-assemblies can be transformed into each other under certain conditions.The regulation of supramolecular self-assembly is not only helpful to understand the self-assembly principle,but also beneficial to its application.In the present study,the self-assembly behavior of epoxy-β-cyclodextrin(EP-β-CD)and mixed anionic and cationic surfactant system(sodium dodecyl sulfate/dodecyltrimethylammonium bromide,SDS/DTAB)in aqueous solution was studied.Morphological and particle size characterization found that the SDS/DTAB@EP-β-CD complex,as the basic building unit,self-assembled into worm-like micelles at lower temperatures and vesicles at higher temperatures.Nuclear magnetic resonance(NMR)and Fourier transform infrared spectroscopy(FT-IR)analysis revealed that the driving force for the formation of vesicles and worm-like micelles was the hydrogen bonds between EP-β-CD molecules,while water molecules played an important role in promoting vesicle formation between SDS/DTAB@EP-β-CD units.Herein,the mechanism of the morphologic transformation of SDS/DTAB@EP-β-CD supramolecular aggregates induced by temperature was elucidated by exploring the self-assembly process,which may provide an excellent basis for the development of delivery carriers.展开更多
In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel ...In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel gelation time are complicated or have low responsiveness.There is an urgent need for an effective method for delaying gel gelation time with intelligent response.Inspired by the slow-release effect of drug capsules,this paper uses the self-assembly effect of gas-phase hydrophobic SiO_(2) in aqueous solution as a capsule to prepare an intelligent responsive self-assembled micro-nanocapsules.The capsule slowly releases the cross-linking agent under the stimulation of external conditions such as temperature and pH value,thus delaying gel gelation time.When the pH value is 2 and the concentration of gas-phase hydrophobic SiO_(2) particles is 10%,the gelation time of the capsule gel system at 30,60,90,and 120℃is12.5,13.2,15.2,and 21.1 times longer than that of the gel system without containing capsule,respectively.Compared with other methods,the yield stress of the gel without containing capsules was 78 Pa,and the yield stress after the addition of capsules was 322 Pa.The intelligent responsive self-assembled micronanocapsules prepared by gas-phase hydrophobic silica nanoparticles can not only delay the gel gelation time,but also increase the gel strength.The slow release of cross-linking agent from capsule provides an effective method for prolongating the gelation time of polymer gels.展开更多
Various ordered mesoporous carbons (OMCs) have been prepared by evaporation-induced trieonstituent co-assembly method. Their mesostructural stability under different carbon content, aging time and acidity were conve...Various ordered mesoporous carbons (OMCs) have been prepared by evaporation-induced trieonstituent co-assembly method. Their mesostructural stability under different carbon content, aging time and acidity were conveniently monitored by X-ray diffraction, transmission electron microscopy, and N2 sorption isotherms techniques. The results show mesostruetural stability of OMCs is enhanced as the carbon content increases from 36% to 46%, further increasing carbon content deteriorates the mesostructural stability. Increasing aging time from 0.5 h to 5.0 h make the mesostructural stability go through an optimum (2.0 h) and gradually reduce framework shrinkage of the OMCs. Highly OMCs can only be obtained in the acidity range of 0.2-1.2 mol/L HC1, when the acidity is near the isoelectrie point of silica, the resulting OMCs have the best mesostructure stability. Under the optimum condition, the carbon content of 46%, aging time of 2.0 h, and 0.2 mol/L HCl, the resulting OMCs have the best mesostrueture stability and the highest BET surface areas of 2281 m2/g.展开更多
A polymerized lyotropic liquid crystal monomer of sodium 3,4,5-tris(11-acryloxyundecyloxy)- benzoate was synthesized by a convenient route starting from 3,4,5-trihydroxybenzoic acid via esterification followed by et...A polymerized lyotropic liquid crystal monomer of sodium 3,4,5-tris(11-acryloxyundecyloxy)- benzoate was synthesized by a convenient route starting from 3,4,5-trihydroxybenzoic acid via esterification followed by etherification, acylation and finally neutralization. The chemi- cal structure was confirmed by Fourier transform infrared (FT-IR) and 1H nuclear magnetic resonance spectral analysis. The self-organization behavior of the monomer with deionized water in methanol at room temperature was also demonstrated. The assemblies were char- acterized by polarized optical microscope and X-ray diffraction. The results show that a solution containing 80:20 of the monomer to water was found to be able to self-organize into Lamellar (La) phase and 92:8 with inverted hexagonal (H]I) phase, which was in ac- cordance with the theoretical calculation of critical packing parameter. It suggests that the concentration of the monomer was the key factor to influence assembly structure. Addi- tionally, the acrylate conversion with different photoinitiators and nanostructure retention after polymerization were investigated. The research shows that the acrylate conversion of the monomer with Darocur2959 could reach up to 78% when irradiated by 30 mW/cm2 UV light of 365 nm for 30 min characterized by Real-time FT-IR as well as the sol-gel method. Meanwhile, the La and HII phase nanostructures were both retained after polymerization.展开更多
基金financially supported by the National Key Research and Development Program of China (2021YFB3600403)the Fundamental Research Funds for the Central Universities (000-0903069032)。
文摘Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.
基金supported by the National Natural Science Foundation of China(22078211)the China Postdoctoral Science Foundation(2022M721115).
文摘The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.
基金National Undergraduate Training Program for Innovation and Entrepreneurship of China (Grant No.202210288027).
文摘The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium alginate-based multilayer film is fabricated via a layer-by-layer(LBL)self-assembly method.With the help of superior interaction between the layers,the multilayer film possesses excellent mechanical properties(with a tensile strength of 50 MPa).Besides,the film displays outstanding water retention property(blocking moisture of 97.56%)and ultraviolet blocking property.Anthocyanin is introduced into the film to detect the food quality since it is one natural plant polyphenol that is sensitive to the pH changes ranging from 1 to 13 in food when spoilage occurs.It is noted that the film is also bacteriostatic which is desired for food packaging.This study describes a simple technique for the development of advanced multifunctional and fully biodegradable food packaging film and it is a sustainable alternative to plastic packaging.
基金Project(ZCLTGS24B0101)supported by Zhejiang Provincial Natural Science Foundation of ChinaProject(Y202250501)supported by Scientific Research Fund of Zhejiang Provincial Education Department,ChinaProject supported by SRT Research Project of Jiaxing Nanhu University,China。
文摘Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.
文摘We consider the inverse problem of finding guiding pattern shapes that result in desired self-assembly morphologies of block copolymer melts.Specifically,we model polymer selfassembly using the self-consistent field theory and derive,in a non-parametric setting,the sensitivity of the dissimilarity between the desired and the actual morphologies to arbitrary perturbations in the guiding pattern shape.The sensitivity is then used for the optimization of the confining pattern shapes such that the dissimilarity between the desired and the actual morphologies is minimized.The efficiency and robustness of the proposed gradient-based algorithm are demonstrated in a number of examples related to templating vertical interconnect accesses(VIA).
基金The work was supported by the National Natural Science Foundation of China(52372174)Carbon Neutrality Research Institute Fund(CNIF20230204)Special Project of Strategic Cooperation between China National Petroleum Corporation and China University of Petroleum(Beijing)(ZLZX-2020-04).
文摘Designing high-performance and low-cost electrocatalysts for oxygen evolu-tion reaction(OER)is critical for the conversion and storage of sustainable energy technologies.Inspired by the biomineralization process,we utilized the phosphorylation sites of collagen molecules to combine with cobalt-based mononuclear precursors at the molecular level and built a three-dimensional(3D)porous hierarchical material through a bottom-up biomimetic self-assembly strategy to obtain single-atom catalysts confined on carbonized biomimetic self-assembled carriers(Co SACs/cBSC)after subsequent high-temperature annealing.In this strategy,the biomolecule improved the anchoring efficiency of the metal precursor through precise functional groups;meanwhile,the binding-then-assembling strategy also effectively suppressed the nonspecific adsorption of metal ions,ultimately preventing atomic agglomeration and achieving strong electronic metal-support interactions(EMSIs).Experimental characterizations confirm that binding forms between cobalt metal and carbonized self-assembled substrate(Co–O_(4)–P).Theoretical calculations disclose that the local environment changes significantly tailored the Co d-band center,and optimized the binding energy of oxygenated intermediates and the energy barrier of oxygen release.As a result,the obtained Co SACs/cBSC catalyst can achieve remarkable OER activity and 24 h durability in 1 M KOH(η10 at 288 mV;Tafel slope of 44 mV dec-1),better than other transition metal-based catalysts and commercial IrO_(2).Overall,we presented a self-assembly strategy to prepare transition metal SACs with strong EMSIs,providing a new avenue for the preparation of efficient catalysts with fine atomic structures.
基金Funded by the Key R&D Program of the Science and Technology Department of Hubei Province(No.2022BCE008)。
文摘Poly(3,4-ethylenedioxyethiophene)-polystyrene sulfonic acid(PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide(PDDA-rGO)was layer by layer self-assembled on the cotton fiber.The surface morphology and electric property was investigated.The results confirmed the dense membrane of PEDOT:PSS and the lamellar structure of PDDA-rGO on the fibers.It has excellent electrical conductivity and mechanical properties.The fiber based electrochemical transistor(FECTs)prepared by the composite conductive fiber has a maximum output current of 8.7 mA,a transconductance peak of 10 mS,an on time of 1.37 s,an off time of 1.6 s and excellent switching stability.Most importantly,the devices by layer by layer self-assembly technology opens a path for the true integration of organic electronics with traditional textile technologies and materials,laying the foundation for their later widespread application.
基金Natural Science Foundation of Tianjin Municipal Science and Technology Commission,Grant/Award Number:20ZYJDJC00040National Natural Science Foundation of China,Grant/Award Numbers:32030084,32202053,U22A20545。
文摘New concept for the development of supramolecular assemblies from intricate inter-actions between different classes of biomacromolecules(polysaccharides,proteins and lipids)is yet to come,due to their intrinsic chemical and structural complex-ity and incompatibility.Herein,we report an interaction mechanism among multiple biomacromolecules,and the structural and digestive properties of their assemblies using amylose(AM),lauric acid(LA),andβ-lactoglobulin(βLG)as exemplars.AM,LA,andβLG interact to form a water-soluble ternary complex through van der Waals forces between AM and LA and high affinity binding between AM andβLG,which can further assemble into uniform-sized,semi-crystalline nanospheres under certain thermodynamic conditions.These nanospheres are substantially resis-tant to amylolysis,thus can be well utilized by gut microbiota,including increasing short-chain fatty acid levels and shaping bacterial communities.Illustrating the com-plexation of AM,LA,andβLG and their assemblies from disorder to order,this work offers potential rationale of assemblies for multiple biomacromolecules driven by non-covalent interactions and substantial potentials for supramolecular biomaterials development.
基金financial supports from National Natural Science Foundation of China(32000992,21977081,32101124)the Zhejiang Provincial Natural Science Foundation for Distinguished Young Scholar(LR23C100001)+1 种基金Wenzhou Medical University(KYYW201901)Zhejiang Qianjiang Talent Plan(QJD20020224)
文摘Ferroptosis has emerged as a potent form of no-apoptotic cell death that offers a promising alternative to avoid the chemoresistance of apoptotic pathways and serves as a vulnerability of cancer.Herein,we have constructed a biomimetic self-assembly nano-prodrug system that enables the co-delivery of gefitinib(Gefi),ferrocene(Fc)and dihydroartemisinin(DHA)for the combined therapy of both ferroptosis and apoptosis.In the tumor microenvironment,this nano-prodrug is able to disassemble and trigger drug release under high levels of GSH.Interestingly,the released DHA can downregulate GPX4 level for the enhancement of intracellular ferroptosis from Fc,further executing tumor cell death with concomitant chemotherapy by Gefi.More importantly,this nano-prodrug provides highly homologous targeting ability by coating related cell membranes and exhibits outstanding inhibition of tumor growth and metastasis,as well as no noticeable side-effects during treatments.This simple small molecular self-assembled nano-prodrug provides a new reasonably designed modality for ferroptosis-combined chemotherapy.
基金The authors gratefully acknowledge the financial support from the National Key R&D Program of China(2021YFC2101304)China Postdoctoral Science Foundation(BX2021041)。
文摘Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;however,the improvement of their energy density remains a challenge.Here,we design a green and universal approach to prepare the composite electrode material,which is composed of lignin-phenolformaldehyde resins derived hierarchical porous carbon(LR-HPC)as conductive skeletons and the self-assembly manganese cobaltite(MnCo_(2)O_(4))nanocrystals as active sites.The synthesized C@MnCo_(2)O_(4)composite has an abundant porous structure and superior electronic conductivity,allowing for more charge/electron mass transfer channels and active sites for the redox reactions.The composite shows excellent electrochemical performance,such as the maximum specific capacitance of~726 mF cm^(-2)at 0.5 mV s^(-1),due to the significantly enhanced interactive interface between LR-HPC and MnCo_(2)O_(4)crystals.The assembled all-solid-state asymmetric supercapacitor,with the LR-HPC and C@MnCo_(2)O_(4)as cathode and anode,respectively,exhibits the highest volumetric energy density of 0.68 mWh cm^(-3)at a power density of 8.2 mW cm^(-3).Moreover,this device shows a high capacity retention ratio of~87.6%at 5 mA cm^(-2)after 5000 cycles.
文摘NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.
基金This work was supported by General Program of National Natural Science Foundation of China(No.816736112017):General Project of Heilongjiang Provincial Science Foundation(No.H2016076)Harbin Special Fund for Scientific and Technological Innovation Talent Research(No.2017RAQXJ090)。
文摘Traditional Chinese medicine decoction is a complex polydispersed phase system containing real solution,colloid solution,emulsion and suspension.The compound decoction of traditional Chinese medicine has complex components,including saponins,alkaloids,polysaccharides,flavonoids,amino acids and so on,which can be self-assembled to form gels,fibers,micelles,vesicles and so on.The self-assembled nano-phase not only neutralizes the single drug and reduces the toxicity and side effects,but also has its own pharmacological effects,which complement each other to achieve synergistic effect,so as to achieve the role of drug supplement,which is of research significance.The formation principle,solubilization and synergism principle and characterization method of multi-component self-assembly of traditional Chinese medicine compound decoction are discussed in this paper.
基金financed by the National Natural Science Foundation of China(52103212)Jiangxi Provincial Natural Science Foundation(20224BAB214022)+7 种基金the SSF Synergy Program(EM16-0004)Swedish Energy Agency(EM 42033-1)the Knut and Alice Wal enberg(KAW)Foundation through a Fellowship Grant and a Project Grant(KAW2020.0033)Support from the National Natural Science Foundation of China(61774077)the Youth Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province(2020A1515110738)the Key Projects of Joint Fund of Basic and Applied Basic Research Fund of Guangdong Province(2019B1515120073)the High-End Foreign Experts Project(G20200019046)the Guangzhou Key laboratory of Vacuum Coating Technologies and New Energy Materials Open Projects Fund(KFVE20200006)
文摘Supercapacitors based on two-dimensional MXene(Ti_(3)C_(2)T_(z))have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance as the thickness increases,caused by increasing ion diffusion limitation.Further limitations include restacking of the nanosheets,which makes it challenging to realize the full potential of these electrode materials.Herein,we demonstrate the design of a vertically aligned MXene hydrogel composite,achieved by thermal-assisted self-assembled gelation,for high-rate energy storage.The highly interconnected MXene network in the hydrogel architecture provides very good electron transport properties,and its vertical ion channel structure facilitates rapid ion transport.The resulting hydrogel electrode show excellent performance in both aqueous and organic electrolytes with respect to high capacitance,stability,and high-rate capability for up to 300μm thick electrodes,which represents a significant step toward practical applications.
基金National Natural Science Foundation of China,Grant/Award Numbers:52275199,82073833,52335004,52022043Beijing-Tianjin-Hebei Fundamental Research Cooperation Project,Grant/Award Number:J230001+1 种基金Hainan Provincial Social Development Fund,Grant/Award Number:ZDYF2023SHFZ145National Key Research and Development Program of China,Grant/Award Numbers:2022YFC3600500,2022YFC3600502。
文摘Myocardial infarction accompanied by diabetes mellitus is accepted as the most seri-ous type of coronary heart disease,and among the current treatment strategies,the precise delivery of protective drugs for inhibiting cardiomyocyte apoptosis is still a challenge.In this study,we developed a biodegradable nanoparticles-based delivery system with excellent macrophage escape,cardiac targeting,and drug release prop-erties to achieve targeted therapy of myocardial infarction.Specifically,a copolymer of p(DMA–MPC–CD)combining self-adhesion,hydration lubrication,and targeting peptide binding site was successfully prepared by free radical copolymerization,and it was self-assembled on the surface of melatonin-loaded dendritic mesoporous silica nanoparticles(bMSNs)following the integration of adamantane-modified cardiac homing peptide(CHP)based on supramolecular host–guest interaction.Importantly,a hydration layer formed around the zwitterionic phosphorylcholine groups of the multifunctional nanoparticles,which was confirmed by the enhancement in hydra-tion lubrication and reduction in coefficient of friction,prevented the nanoparticles from phagocytosis by the macrophages.The in vivo bioluminescence imaging test indicated that the nanoparticles were endowed with satisfied cardiac targeting capa-bility,and the in vivo mice study demonstrated that the intravenous injection of drug-loaded nanoparticles(namely bMSNs–Mel@PDMC–CHP)effectively reduced cardiomyocyte apoptosis,alleviated myocardial interstitialfibrosis,and enhanced cardiac function.
基金supported by the National Natural Science Foundation of China(Grant Nos.62321166653,22090044,and 12350410372).Calculations were performed in part at the high-performance computing center of Jilin University.
文摘Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.
基金Project supported by the National Natural Science Foundation of China (Grants No. 12075201)the Science and Technology Planning Project of Jiangsu Province, China (Grant No. BK20201428)+1 种基金the Postgraduate Research & Practice Innovation Program of Jiangsu Province, China (Grant No. KYCX21 3193)the Special Program for Applied Research on Supercomputation of the NSFC–Guangdong Joint Fund (the second phase)。
文摘The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate strategies for designing anti-fouling surfaces are crucial.Here,we employ molecular dynamics simulations and alchemical free energy calculations to systematically analyze the factors influencing resistance to protein adsorption on the SAMs terminated with single or double OH groups at three packing densities(∑=2.0 nm^(-2),4.5 nm^(-2),and 6.5 nm^(-2)),respectively.For the first time,we observed that the compactness and order of interfacial water enhance its physical barrier effect,subsequently enhancing the resistance of SAM to protein adsorption.Notably,the spatial hindrance effect of SAM leads to the embedding of protein into SAM,resulting in a lack of resistance of SAM towards protein.Furthermore,the number of hydroxyl groups per unit area of double OH-terminated SAM at ∑=6.5 nm^(-2) is approximately 2 to 3 times that of single OH-terminated SAM at ∑=6.5 nm^(-2) and 4.5 nm^(-2),consequently yielding a weaker resistance of double OH-terminated SAM towards protein.Meanwhile,due to the structure of SAM itself,i.e.,the formation of a nearly perfect ice-like hydrogen bond structure,the SAM exhibits the weakest resistance towards protein.This study will complement and improve the mechanism of OH-SAM resistance to protein adsorption,especially the traditional barrier effect of interfacial water.
基金China Postdoctoral Science Foundation(2020M681125)National Natural Science Foundation of China(32272254,31901618)Collaborative Innovation Center of Fragrance Flavour and Cosmetics.
文摘Bio-based cyclodextrins(CDs)are a common research object in supramolecular chemistry.The special cavity structure of CDs can form supramolecular self-assemblies such as vesicles and microcrystals through weak interaction with guest molecules.The different forms of supramolecular self-assemblies can be transformed into each other under certain conditions.The regulation of supramolecular self-assembly is not only helpful to understand the self-assembly principle,but also beneficial to its application.In the present study,the self-assembly behavior of epoxy-β-cyclodextrin(EP-β-CD)and mixed anionic and cationic surfactant system(sodium dodecyl sulfate/dodecyltrimethylammonium bromide,SDS/DTAB)in aqueous solution was studied.Morphological and particle size characterization found that the SDS/DTAB@EP-β-CD complex,as the basic building unit,self-assembled into worm-like micelles at lower temperatures and vesicles at higher temperatures.Nuclear magnetic resonance(NMR)and Fourier transform infrared spectroscopy(FT-IR)analysis revealed that the driving force for the formation of vesicles and worm-like micelles was the hydrogen bonds between EP-β-CD molecules,while water molecules played an important role in promoting vesicle formation between SDS/DTAB@EP-β-CD units.Herein,the mechanism of the morphologic transformation of SDS/DTAB@EP-β-CD supramolecular aggregates induced by temperature was elucidated by exploring the self-assembly process,which may provide an excellent basis for the development of delivery carriers.
基金support and funding from the National Natural Science Foundation of China (No.52174047)Sinopec Project (No.P21063-3)。
文摘In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel gelation time are complicated or have low responsiveness.There is an urgent need for an effective method for delaying gel gelation time with intelligent response.Inspired by the slow-release effect of drug capsules,this paper uses the self-assembly effect of gas-phase hydrophobic SiO_(2) in aqueous solution as a capsule to prepare an intelligent responsive self-assembled micro-nanocapsules.The capsule slowly releases the cross-linking agent under the stimulation of external conditions such as temperature and pH value,thus delaying gel gelation time.When the pH value is 2 and the concentration of gas-phase hydrophobic SiO_(2) particles is 10%,the gelation time of the capsule gel system at 30,60,90,and 120℃is12.5,13.2,15.2,and 21.1 times longer than that of the gel system without containing capsule,respectively.Compared with other methods,the yield stress of the gel without containing capsules was 78 Pa,and the yield stress after the addition of capsules was 322 Pa.The intelligent responsive self-assembled micronanocapsules prepared by gas-phase hydrophobic silica nanoparticles can not only delay the gel gelation time,but also increase the gel strength.The slow release of cross-linking agent from capsule provides an effective method for prolongating the gelation time of polymer gels.
基金This work was supported by the National Natural Science Foundation of China (No.20872135).
文摘Various ordered mesoporous carbons (OMCs) have been prepared by evaporation-induced trieonstituent co-assembly method. Their mesostructural stability under different carbon content, aging time and acidity were conveniently monitored by X-ray diffraction, transmission electron microscopy, and N2 sorption isotherms techniques. The results show mesostruetural stability of OMCs is enhanced as the carbon content increases from 36% to 46%, further increasing carbon content deteriorates the mesostructural stability. Increasing aging time from 0.5 h to 5.0 h make the mesostructural stability go through an optimum (2.0 h) and gradually reduce framework shrinkage of the OMCs. Highly OMCs can only be obtained in the acidity range of 0.2-1.2 mol/L HC1, when the acidity is near the isoelectrie point of silica, the resulting OMCs have the best mesostructure stability. Under the optimum condition, the carbon content of 46%, aging time of 2.0 h, and 0.2 mol/L HCl, the resulting OMCs have the best mesostrueture stability and the highest BET surface areas of 2281 m2/g.
文摘A polymerized lyotropic liquid crystal monomer of sodium 3,4,5-tris(11-acryloxyundecyloxy)- benzoate was synthesized by a convenient route starting from 3,4,5-trihydroxybenzoic acid via esterification followed by etherification, acylation and finally neutralization. The chemi- cal structure was confirmed by Fourier transform infrared (FT-IR) and 1H nuclear magnetic resonance spectral analysis. The self-organization behavior of the monomer with deionized water in methanol at room temperature was also demonstrated. The assemblies were char- acterized by polarized optical microscope and X-ray diffraction. The results show that a solution containing 80:20 of the monomer to water was found to be able to self-organize into Lamellar (La) phase and 92:8 with inverted hexagonal (H]I) phase, which was in ac- cordance with the theoretical calculation of critical packing parameter. It suggests that the concentration of the monomer was the key factor to influence assembly structure. Addi- tionally, the acrylate conversion with different photoinitiators and nanostructure retention after polymerization were investigated. The research shows that the acrylate conversion of the monomer with Darocur2959 could reach up to 78% when irradiated by 30 mW/cm2 UV light of 365 nm for 30 min characterized by Real-time FT-IR as well as the sol-gel method. Meanwhile, the La and HII phase nanostructures were both retained after polymerization.