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Porous ultrathin-shell microcapsules designed by microfluidics for selective permeation and stimuli-triggered release

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1643-1650页

作者： Li Chen Yao Xiao Zhiming Zhang Chun-Xia Zhao Baoling Guo Fangfu Ye Dong Chen Department of Oncology Longyan First Affiliated Hospital of Fujian Medical UniversityLongyan 364000China Zhejiang Key Laboratory of Smart Biomaterials College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Wenzhou Institute University of Chinese Academy of SciencesWenzhou 325001China Faculty of Engineering Computerand Mathematical SciencesThe University of AdelaideAdelaideSA 5005Australia Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China College of Energy Engineering and State Key Laboratory of Fluid Power and Mechatronic Systems Zhejiang UniversityHangzhou 310027China

Microcapsules are versatile delivery vehicles and widely used in various areas.Generally,microcapsules with solid shells lack selective permeation and only exhibit a simple release mode.Here,we use ultrathin-shell water-in-oil-in-water double emulsions as templates and design porous ultrathin-shell microcapsules for selective permeation and multiple stimuli-triggered release.After preparation of double emulsions by microfluidic devices,negatively charged shellac nanoparticles dispersed in the inner water core electrostatically complex with positively charged telechelicα,ω-diamino functionalized polydimethylsiloxane polymers dissolved in the middle oil shell at the water/oil interface,thus forming a porous shell of shellac nanoparticles cross-linked by telechelic polymers.Subsequently,the double emulsions become porous microcapsules upon evaporation of the middle oil phase.The porous ultrathin-shell microcapsules exhibit excellent properties,including tunable size,selective permeation and stimuli-triggered release.Small molecules or particles can diffuse across the shell,while large molecules or particles are encapsulated in the core,and release of the encapsulated cargos can be triggered by osmotic shock or a pH change.Due to their unique performance,porous ultrathin-shell microcapsules present promising platforms for various applications,such as drug delivery.

关键词： microcapsule emulsion microfluidics selective permeation stimuli-triggered release

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Double emulsion-pretreated microwell culture for the in vitro production of multicellular spheroids and their in situ analysis

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Microsystems & Nanoengineering 2021年第3期7卷 73-84页

作者： Fuyang Qu Shirui Zhao Guangyao Cheng Habibur Rahman Qinru Xiao Renee Wan Yi Chan Yi-Ping Ho Department of Biomedical Engineering Faculty of EngineeringThe Chinese University of Hong KongShatinNew TerritoriesHong Kong SARChina CUHK-UMCU Joint Research Laboratory of Respiratory Virus and Immunobiology The Chinese University of Hong KongShatinNew TerritoriesHong Kong SARChina Department of Paediatrics Faculty of MedicineThe Chinese University of Hong KongShatinNew TerritoriesHong Kong SARChina Laboratory for Paediatric Respiratory Research Li Ka Shing Institute of Health SciencesFaculty of MedicineThe Chinese University of Hong KongHong Kong SARChina Hong Kong Hub of Paediatric Excellenee The Chinese University of Hong KongHong Kong SARChina Hong Kong Branch of CAS Center for Excellence in Animal Evolution and Genetics The Chinese University of Hong KongShatinNew TerritoriesHong Kong SARChina The Ministry of Education Key Laboratory of Regeneration Medicine ShatinNew TerritoriesHong Kong SARChina Centre for Novel Biomaterials The Chinese University of Hong KongShatinNew TerritoriesHong Kong SARChina

Multicellular spheroids have served as a promising preclinical model for drug efficacy testing and disease modeling.Many microfluidic tech no logies,in eluding those based on water-oil-water double emulsions,have been introduced for the production of spheroids.However,sustained culture and the in situ characterization of the gen erated spheroids are currently unavailable for the double emulsion-based spheroid model.This study presents a streamlined workflow,termed the double emulsion-pretreated microwell culture(DEPMiC),incorporating the features of(1)effective initiation of uniform-sized multicellular spheroids by the pretreatment of double emulsions produced by microfluidics without the requirement of biomaterial scaffolds;(2)sustained maintenance and culture of the produced spheroids with facile removal of the oil confinement;and(3)in situ characterization of individual spheroids localized in microwells by a built-in analytical station.Characterized by microscopic observations and Raman spectroscopy,the DEPMiC cultivated spheroids accumulated elevated lipid ordering on the apical membran巳similar to that observed in their Matrigel counterparts.Made possible by the proposed tech no logical advancement,this study subsequently examined the drug responses of these in vitro-generated multicellular spheroids.The developed DEPMiC platform is expected to gen erate health benefits in personalized cancer treatment by offering a pre-animal tool to dissect heterogeneity from individual tumor spheroids.

关键词： emulsion sized culture

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MULTI-SCALE STRUCTURES IN emulsion AND MICROSPHERE COMPLEX SYSTEMS

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China Particuology 2005年第6期3卷 296-303页

作者： Guanghui Ma Fangling Gong Guohua Hu Dongxia Ha Rong Liu Renwei Wang National Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Zhongguancun Beijing 100080 P. R. China Laboratory of Chemical Engineering Science CNRS-ENSIC-INPL 1 rue Grandville BP20451 54001 Nancy Cedex France Institut Universitaire de France Maison des University 103 Boulevard Saint-Michel 75005 Pads France

Multi-scale structures involved in emulsion and microsphere complex systems are presented and discussed. The stability and spatio-temporal structures of emulsions, as well as nano-structures formed on the surface of microspheres after polymerization, are affected by the molecular emulsifier/stabilizer structures and the adsorbed emulsifier/stabilizer nano-structures on the oil/water interface. The broad size distribution and variation of surface features of droplets are responsible for variations of the adsorbed emulsifier/stabilizer structures and the stability of the emulsions. On the other hand, preparation of a uniformly sized emulsion and employment of a combined emulsifier/stabilizer system can preserve the stability of the emulsions and microspheres. The above phenomena should be modeled by a multiscale method, in order to maintain the stability of individual emulsion systems and realize the desired nano-structures of microspheres by choosing adequate emulsifier/stabilizer and experimental parameters.

关键词： multi-scale structure spatio-temporal structure emulsion microsphere emulsifier/stabilizer,nano-structure

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BEHAVIOUR OF INHIBITORS IN emulsion POLYMERIZATION(Ⅱ)CaseⅠKinetics

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Chinese Journal of Chemical Engineering 1991年第1期 21-27页

作者： A.Penlidis 霍炳培 MIPPT McMaster Univ.Canada Dept.of Chem.Eng.Univ.of WaterlooOnt.Canada N2L 3G1 Chem.Ind.Res.Inst.of Guangzhou GuangzhouGuangdong

The behaviour of water soluble and monomer soluble inhibitors in the emulsion polymerization for CaseI system(e.***.vinyl acetate and vinyl chloride)has been studied.The behaviour of monomer soluble inhibitorsis shown to be quite different from that observed in Case Ⅱ emulsion polymerization system.Model predictionsof the effect of these inhibitors on polymer particle nucleation and growth rate are shown to be in satisfactoryagreement with experimental results.

关键词： monomer polymerization vinyl emulsion acetate Case Kinetics nucleation behaviour timer

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BEHAVIOUR OF INHIBITORS IN emulsion POLYMERIZATION(Ⅰ)CaseⅡKinetics

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Chinese Journal of Chemical Engineering 1991年第1期 12-20页

作者：霍炳培 A.Penlidis Chem.Ind.Res.Inst.of Guangzhou GuangzhouGuangdong MIPPT McMaster Univ.Canada Department of Chemical EngineeringUniversity of WaterlooWaterlooOntarioCanada N2L 3G1

The behaviour of water soluble and monomer soluble inhibitors in emulsion polymerization of monomersfollowing Case Ⅱ kinetics(e.***.styrene)has been investigated.Experimental studies reveal that inhibitors canhave an appreciable effect on both polymer particle nucleation and growth.A mathematical model showingthese effects has been developed and simulation studies have been done.The simulation results imply that theconsequences of these effects of monomer soluble inhibitors for industrial emulsion polymerization may be quiteserious.

关键词： polymerization monomer emulsion styrene initiator Case Kinetics latex kinetics nucleation

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Self-assembly of colloidal nanoparticles into encapsulated hollow superstructures

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Aggregate 2022年第1期3卷 188-196页

作者： Chaolumen Wu Zhiwei Li Yaocai Bai Dung To Nosang V.Myung Yadong Yin Department of Chemistry University of CaliforniaRiversideCaliforniaUSA Department of Chemical and Biomolecular Engineering University of Notre DameNotre DameIndianaUSA

As a distinct type of nanocapsules,hollow superstructures of inorganic nanoparticles have attracted increasing attention due to their controllable permeability,convenient functionalization,and efficient surface utilization.Conventionally,they are produced by assembling nanoparticles against expensive sacrificial templates.Herein,a general emulsion-based method is reported to assemble colloidal nanoparticles into submicron hollow superstructures,involving first co-assembly of colloidal nanoparticles with organic additives to form clusters,then overcoating the clusters with a polymer shell,and finally removing the organic additives and re-dispersing nanoparticles by exposing to a good solvent.The key to the success of this process is the re-assembly of nanoparticles against the polymer shells as driven by the capillary force during solvent evaporation,producing hollow superstructures.Such a space-confined assembly process can be well controlled by choice of solvents and their evaporation rates.This general technique provides an open and low-cost platform for creating hollow superstructures of various inorganic nanoparticles,offering many opportunities for exploring unique applications that can take advantage of the collective properties of the constituent nanoparticles and the permeable nanoshell structures.

关键词： emulsion hollow superstructures nanoparticles space-confined assembly

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Probing the Interfacial Forces and Surface Interaction Mechanisms in Petroleum Production Processes

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Engineering 2022年第11期18卷 49-61页

作者： Diling Yang Xuwen Peng Qiongyao Peng Tao Wang Chenyu Qiao Ziqian Zhao Lu Gong Yueliang Liu Hao Zhang Hongbo Zeng Department of Chemical and Materials Engineering University of AlbertaEdmontonAB T6G 1H9Canada College of Petroleum Engineering China University of PetroleumBeijing 102249China

Despite the advances that have been made in renewable energy over the past decade,crude oil or petroleum remains one of the most important energy resources to the world.Petroleum production presents many challenging issues,such as the destabilization of complex oil-water emulsions,fouling phenomena on pipelines and other facilities,and water treatment.These problems are influenced by the molecular forces at the oil/water/solid/gas interfaces involved in relevant processes.Herein,we present an overview of recent advances on probing the interfacial forces in several petroleum production processes(e.g.,bitumen extraction,emulsion stabilization and destabilization,fouling and antifouling phenomena,and water treatment)by applying nanomechanical measurement technologies such as a surface forces apparatus(SFA)and an atomic force microscope(AFM).The interaction forces between bitumen and mineral solids or air bubbles in the surrounding fluid media determine the bitumen liberation and flotation efficiency in oil sands production.The stability of complex oil/water emulsions is governed by the forces between emulsion drops and particularly between interface-active species(e.g.,asphaltenes).Various oil components(e.g.,asphaltenes)and emulsion drops interact with different substrate surfaces(e.g.,pipelines or membranes),influencing fouling phenomena,oil-water separation,and wastewater treatment.Quantifying these intermolecular and interfacial forces has advanced the mechanistic understanding of these interfacial interactions,facilitating the development of advanced materials and technologies to solve relevant challenging issues and improve petroleum production processes.Remaining challenges and suggestions on future research directions in the field are also presented.

关键词： Intermolecular and surface forces Interface emulsion Colloids Fouling and antifouling Water treatment

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Electric Field and Ion Diffusion Triggered Precisely Regulated Construction of Micron-scale Water-based Polymer Films:a Detailed Mechanistic Exploration

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Chemical Research in Chinese Universities 2022年第6期38卷 1435-1445页

作者： WANG Dan LIU Jinfang YANG Shuqi JI Xin WANG Yuliang OMONIYI Ahmed Olalekan ZHANG Jianfu SU Zhongmin School of Materials Science and Engineering Changchun University of Science and TechnologyChangchun130022P.R.China School of Chemistry and Environmental Engineering Changchun University of Science and TechnologyChangchun130022P.R.China Jilin Provincial Science and Technology Innovation Center of Optical Materials and Chemistry Changchun University of Science and TechnologyChangchun130022P.R.China

Water-based polymer films can be readily deposited onto a wide range of metallic materials as an environmentally friendly coating through the demulsification-induced fast solidification(DIFS)method.However,there is still a lack of in-depth understanding of the demulsification process of the water-based emulsions and their deposition processes.Herein,we demonstrate that the build-up process of the commercial water-based micron-scale waterborne polyurethane,polyvinyl acetate,polyurethane acrylate,and natural rubber polymer films is affected by the collective effect of electric field and ion diffusion exerted by anode-cathode electrode pairs,applied voltage,conduction time,electrode distance,and emulsion species.A structural investigation of as-prepared polymer films allows us to propose two new structure build-up models.During a flat film deposition,isolated islands are formed first and grow on the substrate surface,and eventually,their mutual coalescence forms the final layer.Whereas,for a convex layer formation,the layer is first formed in the middle of the substrate and then grows toward the sides of the convex structure of the substrate.The results presented in this work expand the understanding of the mechanism of the DIFS process and may provide some new insights into structure-oriented multifunctional material design.

关键词： Polymer film emulsion Demulsification-induced fast solidification Mechanism

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Study on Viscosity Reducing and Oil Displacement Agent for Water-Flooding Heavy Oil Reservoir

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China Petroleum Processing & Petrochemical Technology 2022年第1期24卷 11-18页

作者： Qin Bing Zhao Lin Jiang Jianlin Research Institute of Petroleum Processing SINOPECBeijing 100083

In the process of water-flooding development of heavy oil reservoir,due to the high viscosity and oil-water mobility ratio of heavy oil,there are some problems such as poor fluidity,high residual oil saturation and low recovery efficiency,which seriously restrict the efficient development of heavy oil.The molecular structure characteristics of asphaltenes and resins in heavy oil were analyzed.Based on the three most concerned properties of chemical agents,including the emulsification performance,the interface performance and the oil washing performance,three chemical oil displacement agents for heavy oil reservoirs were developed,and the structure of the chemical agents were characterized by high resolution mass spectrometry.The performance evaluation of chemical agents and core displacement experiments show that there is no obvious correlation between the properties of chemical agents,including interfacial tension,emulsifying ability and oil washing ability.For heavy oil reservoirs,the emulsification and viscosity reduction performance of chemical agents was more important than the oil washing capacity,and the oil washing capacity was more important than the interface performance.Viscosity reduction performance was the key parameter of oil displacement agent suitable for heavy oil reservoir.The composite binary system consisting of the viscosity reducer and the polymer had better oil recovery than using viscosity reducer alone.

关键词： heavy oil viscosity reducer emulsion surfactant enhanced oil recovery

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Building block copolymer particles via self‐assembly within a droplet

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Droplet 2023年第4期2卷 72-90页

作者： Sen Zhang Han Bao Xinyi Shen Yongyang Song Shutao Wang CAS Key Laboratory of Bio‐inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijingChina University of Chinese Academy of Sciences BeijingChina Binzhou Institute of Technology Weiqiao‐UCAS Science and Technology ParkBinzhouChina

The self‐assembly of block copolymers(BCPs)within emulsion droplets is a flexible strategy for the preparation of polymer particles.This strategy permits the finetuning of shapes,internal structures,and surface nanostructures of the polymer particles,thus allowing many applications.Although some literature has reviewed the BCP preparation via self‐assembly within a droplet,a comprehensive summary including in‐depth understanding,controllable preparation,and application is lacked.In this review,we systematically delve into the multiple mechanisms that drive BCP self‐assembly within emulsion droplets,such as commensurability effects for minimizing total free energy,interfacial instability,organized spontaneous emulsification,phase separation of multiple components,and entropy effects between BCPs and nanoparticles.Additionally,a strategy combining selective cross‐linking and disassembly can further generate Janus particles featuring unique structures.Next,various applications across multiple disciplines are discussed,including drug delivery,display,biomedical imaging,macromolecular separation,and fuel cells.Finally,we present an overview of the current challenges and future directions for BCP emulsion self‐assembly,covering mechanism investigation,molecular design,stability control,and application exploration.We anticipate deeper understanding,more varieties,enhanced performance,and broader applications can be achieved with BCP emulsion self‐assembly after addressing the challenge.

关键词： emulsion separation linking

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