Heterostructure particles enable omnidispersible in water and oil towards organic dye recycle.

Dispersion of colloidal particles in water or oil is extensively desired for industrial and environmental applications. However, it often strongly depends on indispensable assistance of chemical surfactants or introduction of nanoprotrusions onto the particle surface. Here we demonstrate the omnidispersity of hydrophilic-hydrophobic heterostructure particles (HL-HBPs), synthesized by a surface heterogeneous nanostructuring strategy. Photo-induced force microscopy (PiFM) and adhesion force images both indicate the heterogeneous distribution of hydrophilic domains and hydrophobic domains on the particle surface. These alternating domains allow HL-HBPs to be dispersed in various solvents with different polarity and boiling point. The HL-HBPs can efficiently adsorb organic dyes from water and release them into organic solvents within several seconds. The surface heterogeneous nanostructuring strategy provides an unconventional approach to achieve omnidispersion of colloidal particles beyond surface modification, and the omnidispersible HL-HBPs demonstrate superior capability for dye recycle merely by solvent exchange. These omnidispersible HL-HBPs show great potentials in industrial process and environmental protection.

Interfacial Polymerization Produced Magnetic Particles with Nano-Filopodia for Highly Accurate Liquid Biopsy in the PSA Gray Zone.

Magnetic particles are leading separation materials for biological purification and detection. Existing magnetic particles, which almost rely on molecule-level interactions, however, often encounter bottlenecks in highly efficient cell-level separation due to the underestimate of surface structure effects. Here, immune cell-inspired magnetic particles with nano-filopodia (NFMPs) produced by interfacial polymerization for highly efficient capture of circulating tumor cells (CTCs) and further accurate clinical diagnosis of prostate cancer are reported . The unprecedented construction of nano-filopodia on polymer-based magnetic particles is achieved by introducing electrostatic interactions in emulsion interfacial polymerization. Due to the unique nano-filopodia, the NFMPs allow remarkably enhanced CTCs capture efficiency (86.5% ± 2.8%) compared with smooth magnetic particles (SMPs, 35.7% ± 5.7%). Under the assistance of machine learning by combining with prostate-specific antigen (PSA) and free to total PSA (F/T-PSA), the NFMPs strategy demonstrates high sensitivity (100%), high specificity (93.3%), and a high area under the curve (AUC) value (98.1%) for clinical diagnosis of prostate cancer in the PSA gray zone. The NFMPs are anticipated as an efficient platform for CTCs-based liquid biopsy toward early cancer diagnosis and prognosis evaluation.

Mediator Monomer Regulated Emulsion Interfacial Polymerization to Synthesize Nanofractal Magnetic Particles for Nucleic Acid Separation.

Polymer-based magnetic particles have been widely used for the separation of biological samples including nucleic acids, proteins, virus, and cells. Existing magnetic particles are almost prepared by coating polymers on magnetic nanoparticles (NPs). However, this strategy usually encounters the problem of poor magnetic NPs loading capacity. Here, a series of nanofractal magnetic particles (nanoFMPs) synthesized by a strategy of mediator monomer regulated emulsion interfacial polymerization is presented, which allows effective magnetic NPs loading and show efficient nucleic acid separation performance. The mediator monomers facilitate the dispersion of magnetic NPs in internal phase to achieve higher loading, and the hydrophilic monomers use electrostatic interactions to form surface nanofractal structures with functional groups. Compared with magnetic particles without nanofractal structure, nanoFMPs exhibit a higher nucleic acid extraction capability. This strategy offers an effective and versatile way for the synthesis of nanoFMPs toward efficient separation in various fields from clinical diagnosis to food safety and environmental monitoring.

Utilizing Heterostructured Porous Particles to Improve Traditional Paper Chromatography for Spontaneous Protein Separation.

Chromatography is a classical technique for protein separation. However, the chromatography column is filled with tightly packed separation materials and requires an additional pressurizing pump to propel the flow of fluidic samples, largely restraining their applications. Here, we combine heterostructured porous particles with paper strips, realizing spontaneous separation of similarly sized proteins. The interconnected nanofibrous structure and good hydrophility of paper strips enable the spontaneous flow of the liquid sample, and the heterostructured porous particles provide versatile tools for protein separation via electrostatic interaction. The fabricated paper strips are inexpensive, user-friendly, and disposable and exhibit good separation performance. This work may offer a new avenue for fabricating on-site bioseparation tools and purifying various biomacromolecules.

Unusual Nanofractal Microparticles for Rapid Protein Capture and Release.

Ion exchange porous microparticles are widely used for protein separation, but their totally porous structure often leads to slow diffusion rate and long separation time. Here unusual nanofractal microparticles synthesized by a strategy of electrostatic interaction regulated emulsion interfacial polymerization are demonstrated that exhibit excellent capability of rapid protein capture, release, and separation. The growth of nanostructures at nanofractal microparticle surface can be controlled by changing electrostatic repulsion between ion groups from weak to strong. The nanofractal microparticles provide a 3D contact model between ion groups and proteins, enable fast protein diffusion rate at initial capture and release stage, and realize rapid and efficient separation of similarly sized proteins as a proof of concept, superior to porous microparticles. This strategy offers an effective and general way for the synthesis of microparticles towards rapid and efficient separation in various fields of biomedicine, environment, and food.

Bioinspired Microfluidic Device by Integrating a Porous Membrane and Heterostructured Nanoporous Particles for Biomolecule Cleaning.

Mimicking the structures and functions of biological systems is considered as a promising approach to construct artificial materials, which have great potential in energy, the environment, and health. Here, we demonstrate a conceptually distinct design by synergistically combining a kidney-inspired porous membrane and natural sponge-inspired heterostructured nanoporous particles to fabricate a bioinspired biomolecule cleaning device, achieving highly efficient biomolecule cleaning spanning from small molecules to macromolecules. The bioinspired biomolecule cleaning device is a two-layer microfluidic device that integrates a polyamide porous membrane and heterostructured nanoporous poly(acrylic acid)-poly(styrene divinylbenzene) particles. The former as a filtration membrane isolates the upper sample liquid and the latter fixed onto the bottom of the underlying channel acts as an active sorbent, particularly enhancing the clearance of macromolecules. As a proof-of-concept, we demonstrate that typical molecules, including urea, creatinine, lysozyme, and ß2-microglobulin, can be efficiently cleaned from simulant liquid and even whole blood. This study provides a method to fabricate a bioinspired biomolecule cleaning device for highly efficient biomolecule cleaning. We believe that our bioinspired synergistic design may expand to other fields for the fabrication of integrated functional devices, creating opportunities in a wide variety of applications.

pH-Regulated Heterostructure Porous Particles Enable Similarly Sized Protein Separation.

Porous particles are frequently used for various healthcare applications that involve protein separation processes. However, conventional porous particles, either homogeneous particles or those subjected to surface modification with a layer of specific molecules, often encounter bottlenecks in separating proteins with similar size. Here, it is reported that heterostructure-enabled separation particles (HESP), synthesized by a double emulsion interfacial polymerization process, can effectively and rapidly separate similarly sized proteins. Double emulsion interfacial polymerization endows the HESP with a nanoscale carboxylic layer outside the particles and inside the pores, allowing pH-regulated selective adsorption of proteins. Thus, by optimizing the environmental pH, proteins with similar size can be effectively and rapidly separated. These HESP are expected to show potential in widespread applications ranging from biomolecule adsorption, encapsulation, and separation to controlled release and other biomedical fields.

Interfacially Polymerized Particles with Heterostructured Nanopores for Glycopeptide Separation.

Porous polymer materials are extensively used for biomolecule separation. However, conventional homogeneous porous polymer materials cannot efficiently separate specific low-abundance biomolecules from complex samples. Here, particles fabricated by emulsion interfacial polymerization featuring heterostructured nanopores with tunable size are reported, which can be used to realize low-abundance glycopeptide (GP) separation from complex biofluids. The heterostructured surface inside the nanopores allows solvent-dependent local adsorption of biomolecules onto hydrophilic or hydrophobic regions. Low-abundance hydrophilic GPs in complex biofluids can be efficiently separated via the hydrophilic region of nanopores in low-polarity solvent after the hydrophobic region removes high-abundance hydrophobic proteins and non-glycopeptides in high-polarity solvent. It is expected that these particles with heterostructured nanopores can be used for separation of nucleic acids, saccharides, and proteins, and downstream clinical diagnosis.

A general strategy to synthesize chemically and topologically anisotropic Janus particles.

Emulsion polymerization is the most widely used synthetic technique for fabricating polymeric particles. The interfacial tension generated with this technique limits the ability to tune the topology and chemistry of the resultant particles. We demonstrate a general emulsion interfacial polymerization approach that involves introduction of additional anchoring molecules surrounding the microdroplets to synthesize a large variety of Janus particles with controllable topological and chemical anisotropy. This strategy is based on interfacial polymerization mediated by an anchoring effect at the interface of microdroplets. Along the interface of the microdroplets, the diverse topology and surface chemistry features of the Janus particles can be precisely tuned by regulating the monomer type and concentration as well as polymerization time. This method is applicable to a wide variety of monomers, including positively charged, neutrally charged, and negatively charged monomers, thereby enriching the community of Janus particles.

Controllable drug release and effective intracellular accumulation highlighted by anisotropic biodegradable PLGE nanoparticles.

Control of the stretching or compressing ratio of spherical nanoparticles (NPs) leads to a dramatic change in the shape and size of particles based on amphiphilic biodegradable poly(lactide-co-glycolide-b-ethylene glycol-b-lactide-co-glycolide) (PLGE) triblock copolymers. Drug release, endocytosis and intracellular accumulation tests on these anisotropic PLGE NPs show significantly enhanced properties in comparison with spherical NPs, indicating they are good candidates for drug delivery.