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1.
Nature ; 627(8005): 763-766, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38538938

RESUMO

Relativistic jets are observed from accreting and cataclysmic transients throughout the Universe, and have a profound impact on their surroundings1,2. Despite their importance, their launch mechanism is not known. For accreting neutron stars, the speed of their compact jets can reveal whether the jets are powered by magnetic fields anchored in the accretion flow3 or in the star itself4,5, but so far no such measurements exist. These objects can show bright explosions on their surface due to unstable thermonuclear burning of recently accreted material, called type-I X-ray bursts6, during which the mass-accretion rate increases7-9. Here, we report on bright flares in the jet emission for a few minutes after each X-ray burst, attributed to the increased accretion rate. With these flares, we measure the speed of a neutron star compact jet to be v = 0.38 - 0.08 + 0.11 c , much slower than those from black holes at similar luminosities. This discovery provides a powerful new tool in which we can determine the role that individual system properties have on the jet speed, revealing the dominant jet launching mechanism.

2.
Nature ; 592(7855): 558-563, 2021 04.
Artigo em Inglês | MEDLINE | ID: mdl-33883730

RESUMO

Successfully interfacing enzymes and biomachinery with polymers affords on-demand modification and/or programmable degradation during the manufacture, utilization and disposal of plastics, but requires controlled biocatalysis in solid matrices with macromolecular substrates1-7. Embedding enzyme microparticles speeds up polyester degradation, but compromises host properties and unintentionally accelerates the formation of microplastics with partial polymer degradation6,8,9. Here we show that by nanoscopically dispersing enzymes with deep active sites, semi-crystalline polyesters can be degraded primarily via chain-end-mediated processive depolymerization with programmable latency and material integrity, akin to polyadenylation-induced messenger RNA decay10. It is also feasible to achieve processivity with enzymes that have surface-exposed active sites by engineering enzyme-protectant-polymer complexes. Poly(caprolactone) and poly(lactic acid) containing less than 2 weight per cent enzymes are depolymerized in days, with up to 98 per cent polymer-to-small-molecule conversion in standard soil composts and household tap water, completely eliminating current needs to separate and landfill their products in compost facilities. Furthermore, oxidases embedded in polyolefins retain their activities. However, hydrocarbon polymers do not closely associate with enzymes, as their polyester counterparts do, and the reactive radicals that are generated cannot chemically modify the macromolecular host. This study provides molecular guidance towards enzyme-polymer pairing and the selection of enzyme protectants to modulate substrate selectivity and optimize biocatalytic pathways. The results also highlight the need for in-depth research in solid-state enzymology, especially in multi-step enzymatic cascades, to tackle chemically dormant substrates without creating secondary environmental contamination and/or biosafety concerns.


Assuntos
Lipase/metabolismo , Nanotecnologia , Poliésteres/química , Poliésteres/metabolismo , Polimerização , Biocatálise , Domínio Catalítico , Estabilidade Enzimática , Cinética , Oxirredutases/metabolismo , Polienos/química , Polienos/metabolismo , Especificidade por Substrato
3.
Proc Natl Acad Sci U S A ; 120(28): e2302907120, 2023 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-37399425

RESUMO

Millifluidics, the manipulation of liquid flow in millimeter-sized channels, has been a revolutionary concept in chemical processing and engineering. The solid channels that contain the liquids, though, are not flexible in their design and modification, and prevent contact with the external environment. All-liquid constructs, on the other hand, while flexible and open, are imbedded in a liquid environment. Here, we provide a route to circumvent these limitations by encasing the liquids in a hydrophobic powder in air that jams on the surface, containing and isolating flowing fluids, offering flexibility and adaptability in design, as manifest in the ability to reconfigure, graft, and segment the constructs. Along with the open nature of these powder-contained channels that allow arbitrary connections/disconnections and substance addition/extraction, numerous applications can be opened in the biological, chemical, and material arenas.

4.
Nature ; 569(7756): 374-377, 2019 05.
Artigo em Inglês | MEDLINE | ID: mdl-31036949

RESUMO

Powerful relativistic jets are one of the main ways in which accreting black holes provide kinetic feedback to their surroundings. Jets launched from or redirected by the accretion flow that powers them are expected to be affected by the dynamics of the flow, which for accreting stellar-mass black holes has shown evidence for precession1 due to frame-dragging effects that occur when the black-hole spin axis is misaligned with the orbital plane of its companion star2. Recently, theoretical simulations have suggested that the jets can exert an additional torque on the accretion flow3, although the interplay between the dynamics of the accretion flow and the launching of the jets is not yet understood. Here we report a rapidly changing jet orientation-on a time scale of minutes to hours-in the black-hole X-ray binary V404 Cygni, detected with very-long-baseline interferometry during the peak of its 2015 outburst. We show that this changing jet orientation can be modelled as the Lense-Thirring precession of a vertically extended slim disk that arises from the super-Eddington accretion rate4. Our findings suggest that the dynamics of the precessing inner accretion disk could play a role in either directly launching or redirecting the jets within the inner few hundred gravitational radii. Similar dynamics should be expected in any strongly accreting black hole whose spin is misaligned with the inflowing gas, both affecting the observational characteristics of the jets and distributing the black-hole feedback more uniformly over the surrounding environment5,6.

5.
J Am Chem Soc ; 146(12): 8189-8197, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38471087

RESUMO

Conventional ligands for CsPbBr3 perovskite nanocrystals (NCs), composed of polar, coordinating head groups (e.g., ammonium or zwitterionic) and aliphatic tails, are instrumental in stabilizing the NCs against sintering and aggregation. Nonetheless, the aliphatic (insulating) nature of these ligands represents drawbacks with respect to objectives in optoelectronics, and yet removing these ligands typically leads to a loss of colloidal stability. In this paper, we describe the preparation of CsPbBr3 NCs in the presence of discrete conjugated oligomers that were prepared by an iterative synthetic approach and capped at their chain ends with sulfobetaine zwitterions for perovskite coordination. Notably, these zwitterionic oligofluorenes are compatible with the hot injection and ligand exchange conditions used to prepare CsPbBr3 NCs, yielding stable NC dispersions with high photoluminescence quantum yields (PLQY, >90%) and spectral features representative of both the perovskite core and conjugated ligand shell. Controlling the chain length of these capping ligands effectively regulated inter-NC spacing and packing geometry when cast into solid films, with evidence derived from both transmission electron microscopy (TEM) and grazing incidence X-ray scattering measurements.

6.
J Am Chem Soc ; 146(19): 13000-13009, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38710503

RESUMO

Amphiphilic bottlebrush block copolymers (BBCPs), having a hydrophilic bottlebrush polymer (BP) linked covalently to a hydrophobic BP, were found to segregate to liquid-liquid interfaces to minimize the free energy of the system. The key parameter influencing the outcome of the experiments is the ratio between the degree of polymerization of the backbone (NBB) and that of the side-chain brushes (NSC). Specifically, a spherical, star-like configuration results when NBB < NSC, while a cylindrical, bottlebrush-like shape is preferred when NBB > NSC. Dynamic interfacial tension (γ) and fluorescence recovery after photobleaching (FRAP) measurements show that the BBCP configuration influences the areal density and in-plane diffusion at the fluid interface. The characteristic relaxation times associated with BBCP adsorption (τA) and reorganization (τR) were determined by fitting time-dependent interfacial tension measurements to a sum of two exponential relaxation functions. Both τA and τR initially increased with NBB up to 92 repeat units, due to the larger hydrodynamic radius in solution and slower in-plane diffusivity, attributed to a shorter cross-sectional diameter of the side-chains near the block junction. This trend reversed at NBB = 190, with shorter τA and τR attributed to increased segregation strength and exposure of the bare water/toluene interface due to tilting and/or wiggling of the backbone chains, respectively. The adsorption energy barrier decreased with higher NBB, due to a reduced BBCP packing density at the fluid interface. This study provides fundamental insights into macromolecular assembly at fluid interfaces, as it pertains to unique bottlebrush block architectures.

7.
Small ; : e2312275, 2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38573924

RESUMO

High internal phase emulsions (HIPEs) have been of great interest for fabricating fluorinated porous polymers having controlled pore structures and excellent physicochemical properties. However, it remains a challenge to prepare stable fluorocarbon HIPEs, due to the lack of suitable surfactants. By randomly grating hydrophilic and fluorophilic side chains to polyphosphazene (PPZ), a comb-like amphiphilic PPZ surfactant with biodegradability is designed and synthesized for stabilizing water/fluorocarbon oil-based emulsions. The hydrophilic-lipophilic balance of PPZs can be controlled by tuning the grating ratio of the two side chains, leading to the preparation of stable water-in-oil HIPEs and oil-in-water emulsions, and the production of fluorinated porous polymers and particles by polymerizing the oil phase. These fluorinated porous polymers show excellent thermal stability and, due to the hydrophobicity and porous structure, applications in the field of oil/water separation can be achieved.

8.
Small ; 20(15): e2308560, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-37994305

RESUMO

The in-plane packing of gold (Au), polystyrene (PS), and silica (SiO2) spherical nanoparticle (NP) mixtures at a water-oil interface is investigated in situ by UV-vis reflection spectroscopy. All NPs are functionalized with carboxylic acid such that they strongly interact with amine-functionalized ligands dissolved in an immiscible oil phase at the fluid interface. This interaction markedly increases the binding energy of these nanoparticle surfactants (NPSs). The separation distance between the Au NPSs and Au surface coverage are measured by the maximum plasmonic wavelength (λmax) and integrated intensities as the assemblies saturate for different concentrations of non-plasmonic (PS/SiO2) NPs. As the PS/SiO2 content increases, the time to reach intimate Au NP contact also increases, resulting from their hindered mobility. λmax changes within the first few minutes of adsorption due to weak attractive inter-NP forces. Additionally, a sharper peak in the reflection spectrum at NP saturation reveals tighter Au NP packing for assemblies with intermediate non-plasmonic NP content. Grazing incidence small angle X-ray scattering (GISAXS) and scanning electron microscopy (SEM) measurements confirm a decrease in Au NP domain size for mixtures with larger non-plasmonic NP content. The results demonstrate a simple means to probe interfacial phase separation behavior using in situ spectroscopy as interfacial structures densify into jammed, phase-separated NP films.

9.
Soft Matter ; 20(7): 1554-1564, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38270211

RESUMO

Bottlebrush random copolymers (BRCPs), consisting of a random distribution of two homopolymer chains along a backbone, can segregate to the interface between two immiscible homopolymers. BRCPs undergo a reconfiguration, where each block segregates to one of the homopolymer phases, adopting a Janus-type structure, reducing the interfacial tension and promoting adhesion between the two homopolymers, thereby serving as a Janus bottlebrush copolymer (JBCP) compatibilizer. We synthesized a series of JBCPs by copolymerizing deuterated or hydrogenated polystyrene (DPS/PS) and poly(tert-butyl acrylate) (PtBA) macromonomers using ruthenium benzylidene-initiated ring-opening metathesis polymerization (ROMP). Subsequent acid-catalyzed hydrolysis converted the PtBA brushes to poly(acrylic acid) (PAA). The JBCPs were then placed at the interface between DPS/PS homopolymers and poly(2-vinyl pyridine) (P2VP) homopolymers, where the degree of polymerization of the backbone (NBB) and the grafting density (GD) of the JBCPs were varied. Neutron reflectivity (NR) was used to determine the interfacial width and segmental density distributions (including PS homopolymer, PS block, PAA block and P2VP homopolymer) across the polymer-polymer interface. Our findings indicate that the star-like JBCP with NBB = 6 produces the largest interfacial broadening. Increasing NBB to 100 (rod-like shape) and 250 (worm-like shape) reduced the interfacial broadening due to a decrease in the interactions between blocks and homopolymers by stretching of blocks. Decreasing the GD from 100% to 80% at NBB = 100 caused an increase the interfacial width, yet further decreasing the GD to 50% and 20% reduced the interfacial width, as 80% of GD may efficiently increase the flexibility of blocks and promote interactions between homopolymers, while maintaining relatively high number of blocks attached to one molecule. The interfacial conformation of JBCPs was further translated into compatibilization efficiency. Thin film morphology studies showed that only the lower NBB values (NBB = 6 and NBB = 24) and the 80% GD of NBB = 100 had bicontinuous morphologies, due to a sufficient binding energy that arrested phase separation, supported by mechanical testing using asymmetric double cantilever beam (ADCB) tests. These provide fundamental insights into the assembly behavior of JBCPs compatibilizers at homopolymer interfaces, opening strategies for the design of new BCP compatibilizers.

10.
Proc Natl Acad Sci U S A ; 118(8)2021 02 23.
Artigo em Inglês | MEDLINE | ID: mdl-33602813

RESUMO

The assembly and jamming of magnetic nanoparticles (NPs) at liquid-liquid interfaces is a versatile platform to endow structured liquid droplets with a magnetization, i.e., producing ferromagnetic liquid droplets (FMLDs). Here, we use hydrodynamics experiments to probe how the magnetization of FMLDs and their response to external stimuli can be tuned by chemical, structural, and magnetic means. The remanent magnetization stems from magnetic NPs jammed at the liquid-liquid interface and dispersed NPs magneto-statically coupled to the interface. FMLDs form even at low concentrations of magnetic NPs when mixing nonmagnetic and magnetic NPs, since the underlying magnetic dipole-driven clustering of magnetic NP-surfactants at the interface produces local magnetic properties, similar to those found with pure magnetic NP solutions. While the net magnetization is smaller, such a clustering of NPs may enable structured liquids with heterogeneous surfaces.

11.
Nano Lett ; 23(1): 155-162, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36562701

RESUMO

The direct 3D printing of ultralight architectures with ultralow-concentration 2D nanomaterial inks is necessary yet challenging. Here, we describe an emulsion-based ink for direct printing using 2D nanomaterials, i.e., MXene and graphene oxide (GO). The electrostatic interactions between the ligands in the oil phase and the 2D nanomaterials in the aqueous phase help form sheet-like surfactants at the interface. The interactions between the anchored ligands among different droplets dictate the rheological characteristics of inks, enabling a gel-like behavior ideally suitable for 3D printing at ultralow concentrations of 2D nanomaterials. The 3D printed foams possess lightweight structures with densities of 2.8 mg cm-3 (GO-based) and 4.1 mg cm-3 (MXene-based), and the latter integrates outstanding electrical conductivity, electromagnetic shielding performance, and thermal insulation comparable to air. This work describes a general approach for direct-printing ultralight porous structures that take advantage of the inherent properties of 2D building blocks.

12.
Nano Lett ; 23(22): 10383-10390, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37955362

RESUMO

Nearly monodisperse nanoparticle (NP) spheres attached to a nonvolatile ionic liquid surface were tracked by in situ scanning electron microscopy to obtain the tracer diffusion coefficient Dtr as a function of the areal fraction ϕ. The in situ technique resolved both tracer (gold) and background (silica) particles for ∼1-2 min, highlighting their mechanisms of diffusion, which were strongly dependent on ϕ. Structure and dynamics at low and moderate ϕ paralleled those reported for larger colloidal spheres, showing an increase in order and a decrease in Dtr by over 4 orders of magnitude. However, ligand interactions were more important near jamming, leading to different caging and jamming dynamics for smaller NPs. The normalized Dtr at ultrahigh ϕ depended on particle diameter and ligand molecular weight. Increasing the PEG molecular weight by a factor of 4 increased Dtr by 2 orders of magnitude at ultrahigh ϕ, indicating stronger ligand lubrication for smaller particles.

13.
HPB (Oxford) ; 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38755085

RESUMO

BACKGROUND: Diabetes mellitus (DM) has a complex relationship with pancreatic cancer. This study examines the impact of preoperative DM, both recent-onset and pre-existing, on long-term outcomes following pancreatoduodenectomy (PD) for pancreatic ductal adenocarcinoma (PDAC). METHODS: Data were extracted from the Recurrence After Whipple's (RAW) study, a multi-centre cohort of PD for pancreatic head malignancy (2012-2015). Recurrence and five-year survival rates of patients with DM were compared to those without, and subgroup analysis performed to compare patients with recent-onset DM (less than one year) to patients with established DM. RESULTS: Out of 758 patients included, 187 (24.7%) had DM, of whom, 47 of the 187 (25.1%) had recent-onset DM. There was no difference in the rate of postoperative pancreatic fistula (DM: 5.9% vs no DM 9.8%; p = 0.11), five-year survival (DM: 24.1% vs no DM: 22.9%; p = 0.77) or five-year recurrence (DM: 71.7% vs no DM: 67.4%; p = 0.32). There was also no difference between patients with recent-onset DM and patients with established DM in postoperative outcomes, recurrence, or survival. CONCLUSION: We found no difference in five-year recurrence and survival between diabetic patients and those without diabetes. Patients with pre-existing DM should be evaluated for PD on a comparable basis to non-diabetic patients.

14.
Angew Chem Int Ed Engl ; 63(11): e202400127, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38206892

RESUMO

The phase behavior of block copolymers (BCPs) at the water-oil interface is influenced by the segmental interaction parameter ( χ ${\chi }$ ) and chain architecture. We synthesized a series of star block copolymers (s-BCPs) having polystyrene (PS) as core and poly(2-vinylpyridine) (P2VP) as corona. The interaction parameters of block-block ( χ ${\chi }$ PS-P2VP ) and block-solvent ( χ ${\chi }$ P2VP-solvent ) were varied by adjusting the pH of the aqueous solution. Lowering pH increased the fraction of quaternized-P2VP (Q-P2VP) with enhanced hydrophilicity. By transferring the equilibrated interfacial assemblies, morphologies ranging from bicontinuous films at pH of 7 and 3.1 to nanoporous and nanotubular structure at pH of 0.65 were observed. The nanoporous films formed hexagonally packed pores in s-BCP matrix, while nanotubes comprised Q-P2VP as corona and PS as core. Control over pore size, d-spacing between pores, and nanotube diameters was achieved by varying polymer concentration, molecular weight, volume fraction and arm number of s-BCPs. Large-scale nanoporous films were obtained by freeze-drying emulsions. Remarkably, the morphologies of linear BCPs were inverted, forming hexagonal-packed rigid spherical micelles with Q-P2VP as core and PS as corona in multilayer. This work provides insights of phase behaviors of BCP at fluids interface and offer a facile approach to prepare nanoporous film with well-controlled pore structure.

15.
Angew Chem Int Ed Engl ; 63(25): e202404382, 2024 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-38616164

RESUMO

We formed core-shell-like polyelectrolyte complexes (PECs) from an anionic bottlebrush polymer with poly (acrylic acid) side chains with a cationic linear poly (allylamine hydrochloride). By varying the pH, the number of side chains of the polyanionic BB polymers (Nbb), the charge density of the polyelectrolytes, and the salt concentration, the phase separation behavior and salt resistance of the complexes could be tuned by the conformation of the BBs. By combining the linear/bottlebrush polyelectrolyte complexation with all-liquid 3D printing, flow-through tubular constructs were produced that showed selective transport across the PEC membrane comprising the walls of the tubules. These tubular constructs afford a new platform for flow-through delivery systems.

16.
Angew Chem Int Ed Engl ; 63(24): e202403790, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38589294

RESUMO

Assemblies of nanoparticles at liquid interfaces hold promise as dynamic "active" systems when there are convenient methods to drive the system out of equilibrium via crowding. To this end, we show that oversaturated assemblies of charged nanoparticles can be realized and held in that state with an external electric field. Upon removal of the field, strong interparticle repulsive forces cause a high in-plane electrostatic pressure that is released in an explosive emulsification. We quantify the packing of the assembly as it is driven into the oversaturated state under an applied electric field. Physiochemical conditions substantially affect the intensity of the induced explosive emulsification, underscoring the crucial role of interparticle electrostatic repulsion.

17.
J Am Chem Soc ; 145(46): 25431-25439, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37955662

RESUMO

Reversible Pickering emulsions, achieved by switchable, interfacially active colloidal particles, that enable on-demand emulsification/demulsification or phase inversion, hold substantial promise for biphasic catalysis, emulsion polymerization, cutting fluids, and crude oil pipeline transportation. However, particles with such a responsive behavior usually require complex chemical syntheses and surface modifications, limiting their extensive use. Herein, we report a simple route to generate emulsions that can be controlled and reversibly undergo phase inversion. The emulsions are prepared and stabilized by the interfacial assembly of polyoxometalate (POM)-polymer, where their electrostatic interaction at the interface is dynamic. The wettability of the POMs that dictates the emulsion type can be readily regulated by tuning the number of polymer chains bound to POMs, which, in turn, can be controlled by varying the concentrations of both components and the water/oil ratio. In addition, the number of polymer chains anchored to the POMs can be varied by controlling the number of negative charges on the POMs through an in situ redox reaction. As such, a reversible inversion of the emulsions can be triggered by switching between exposure to ultraviolet light and the introduction of oxygen. Combining the functions of POM itself, a cyclic interfacial catalysis system was realized. Inversion of the emulsion also affords a pathway to high-internal-phase emulsions. The diversity of the POMs, the polymers, and the responsive switching groups open numerous new, simple strategies for designing a wide range of responsive soft matter for cargo loading, controlled release, and delivery in biomedical and engineering applications without time-consuming particle syntheses.

18.
Acc Chem Res ; 55(8): 1097-1108, 2022 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-35188380

RESUMO

ConspectusOrganic photovoltaics (OPVs) have the advantages of being lightweight, mechanically flexible, and solution-processable over large areas, and for decades, they have been the focus of the academic and industrial communities. Recent progress in the design of high-performance organic semiconductors and device optimization has promoted solar cell efficiencies of up to 19%, showing great promise for commercialization. Optimally designed OPVs are achieved using a bicontinuous interpenetrating network of donor and acceptor materials in between two charge-collecting electrodes. Charge extraction and transport between metal electrodes and organic semiconductors are crucial to device operation. The energy-level mismatch when metal electrodes and organic semiconductors are in contact usually induces additional energy barriers and resultant inefficient charge transport and collection, leading to charge carrier recombination at the interface and inferior device performance. To align energy levels at the interface, interlayer materials and their integration into devices have emerged as a widely used strategy to promote the performance of solar cell devices. Interlayer materials have the ability to modify the work functions (WFs) of metal electrodes, holding the potential to enhance the built-in electrostatic field (Vbi) of the devices and suppress the charge recombination loss, which is beneficial to improving the open circuit voltage (VOC), short circuit current density (JSC), and fill factor (FF) of the solar cells.Organic interlayer materials have recently come into focus for fundamental study and practical development because of their diverse molecular design and superior solution processability. Tremendous effort has been devoted to exploring novel organic interlayer materials to achieve all-solution-processed multilayer solar cells. Such interlayer materials usually have orthogonal solubilities relative to the photoactive layer materials, working as multifunctional interfacial layers to manipulate the mechanical and electrical contacts in solar cell devices. Ionenes are a unique class of polyelectrolytes wherein the ionic species reside within the polymer backbone rather than as pendant groups. In ionenes, the charge density is high in comparison to that of other polyelectrolytes, and the periodicity of the charges is easily controlled, providing a tunable density of dipole moments. Ionenes can be readily synthesized from 3° diamines and α,ω-dihaloalkanes to generate polymer chains of ammonium cations connected by flexible hydrocarbon linkages with mobile anions. However, the requisite building blocks of ionenes are not limited to such molecules. Recent advances in combining ionenes with conjugated molecules to generate electroactive ionenes have catalyzed a great amount of interest in such polymers for organic electronic devices.In this Account, we first introduce the molecular design and synthesis of electroactive ionenes. Following this, we will discuss the mechanism and effect of ionenes on the modification of metal electrodes. We then review the strategies for controlling the morphology of ionene interlayers. Finally, we compare the doping effect, conductivity, and charge transport of some representative ionenes and their performance as interlayers in solar cell devices. We present our current understanding based on recent progress and outstanding issues of interlayer materials in OPVs and to propose future directions and opportunities.

19.
Proc Natl Acad Sci U S A ; 117(15): 8360-8365, 2020 04 14.
Artigo em Inglês | MEDLINE | ID: mdl-32220955

RESUMO

Natural and man-made robotic systems use the interfacial tension between two fluids to support dense objects on liquid surfaces. Here, we show that coacervate-encased droplets of an aqueous polymer solution can be hung from the surface of a less dense aqueous polymer solution using surface tension. The forces acting on and the shapes of the hanging droplets can be controlled. Sacs with homogeneous and heterogeneous surfaces are hung from the surface and, by capillary forces, form well-ordered arrays. Locomotion and rotation can be achieved by embedding magnetic microparticles within the assemblies. Direct contact of the droplet with air enables in situ manipulation and compartmentalized cascading chemical reactions with selective transport. Applications including functional microreactors, motors, and biomimetic robots are evident.

20.
Nano Lett ; 22(13): 5538-5543, 2022 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-35766622

RESUMO

Ferrofluids (FFs) can adapt their shape to a magnetic field. However, they cannot maintain their shape when the magnetic field is removed. Here, with a magneto-responsive and reconfigurable interfacial self-assembly (MRRIS) process, we show that FFs can be structured by a magnetic field and maintain their shape, like solids, after removing the magnetic field. The competing self-assembly of magnetic and nonmagnetic nanoparticles at the liquid interface endow FFs with both reconfigurability and structural stability. By manipulating the external magnetic field, we show that it is possible to "write" and "erase" the shape of the FFs remotely and repeatedly. To gain an in-depth understanding of the effect of MRRIS on the structure of FFs, we systematically study the shape variation of these liquids under both the static and dynamic magnetic fields. Our study provides a simple yet novel way of manipulating FFs and opens opportunities for the fabrication of all-liquid devices.


Assuntos
Coloides , Nanopartículas , Coloides/química , Campos Magnéticos , Magnetismo , Nanopartículas/química
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