PNIPAM Shell Research Articles

Temperature-sensitive metal-enhanced fluorescence and plasmon resonance energy transfer.

Experimental decoupling of the effects of plasmon resonance energy transfer (PRET) and metal-enhanced fluorescence (MEF) within the same nanometal-fluorophore pair is fascinating but challenging. In this study, we presented a possible solution for this by coating plasmonic Au nanoparticles (AuNPs) with temperature-sensitive poly(N-isopropylacrylamide) (pNIPAM) shells and R6G hybrids, termed the Au@p-R nanoplatform, which could reversibly adjust the separation between dyes and the AuNP surface, enabling an ON/OFF switch between MEF and PRET. In our optimization process, we discovered that 20 kDa of pNIPAM causes an MEF effect owing to an appropriate shrinking distance of 6.86 ± 0.85 nm. This dual-model nanoplatform exhibits great potential for tracking temperature-dependent transitions.

Collagen-Binding Nanoparticles for Paclitaxel Encapsulation and Breast Cancer Treatment.

In this study, we developed a novel hybrid collagen-binding nanocarrier for potential intraductal administration and local breast cancer treatment. The particles were formed by the encapsulation of nanostructured lipid carriers (NLCs) containing the cytotoxic drug paclitaxel within a shell of poly(N-isopropylacrylamide) (pNIPAM), and were functionalized with SILY, a peptide that binds to collagen type I (which is overexpressed in the mammary tumor microenvironment) to improve local retention and selectivity. The encapsulation of the NLCs in the pNIPAM shell increased nanoparticle size by approximately 140 nm, and after purification, a homogeneous system of hybrid nanoparticles (∼96%) was obtained. The nanoparticles exhibited high loading efficiency (<76%) and were capable of prolonging paclitaxel release for up to 120 h. SILY-modified nanoparticles showed the ability to bind to collagen-coated surfaces and naturally elaborated collagen. Hybrid nanoparticles presented cytotoxicity up to 3.7-fold higher than pNIPAM-only nanoparticles on mammary tumor cells cultured in monolayers. In spheroids, the increase in cytotoxicity was up to 1.8-fold. Compared to lipid nanoparticles, the hybrid nanoparticle modified with SILY increased the viability of nontumor breast cells by up to 1.59-fold in a coculture model, suggesting the effectiveness and safety of the system.

Dual Stimuli‐Responsive Ternary Core‐Shell Polystyrene@Pnipam‐Pedot Latexes

AbstractThe ability of stimuli‐responsive materials to respond to external stimuli depends on their intra‐ and intermolecular interactions, which, in turn, are governed by changes in the material composition. Here, the importance of these factors for new heat and light‐sensitive latexes of core‐shell nanoparticles is reported with the polystyrene core, the poly(N‐isopropylacrylamide) (PNIPAM) shell containing doped poly(3,4‐ethylenedioxythiophene) (PEDOT). It is found that hydrogen bonding, C═O─π aromatic, hydrophilic‐hydrophobic interactions in the shell cause conformational changes in PNIPAM similar to those occurring in the PNIPAM coil‐globule transition. Depending on the EDOT:PS@PNIPAM feed ratio and the PEDOT content in PNIPAM shells, these interactions and changes affect nanoparticle sizes and are responsible for shifting the lower critical solution temperature (LCST) of PNIPAM in the shell from 32.1 to 33.9 °C. The core‐shell morphology of nanoparticles is maintained only for latexes with EDOT feed to ≈9 wt.%. At the higher EDOT content, PNIPAM shells are destroyed. Synthesized PS@PNIPAM‐PEDOT latexes demonstrate temperature‐dependent behavior and produce a photothermal effect under NIR irradiation, which allows for a rise of their temperature above LCST. This dual stimuli (heat and light) responsiveness suggests an important possibility for these latexes to be used for drug or diagnostic agent delivery.

A smart gating nanocellulose membrane showing selective separation and self-cleaning performance

A smart gating membrane based on thermal-sensitive poly (N-isopropyl acrylamide) (PNIPAM)-grafted nanocellulose and carbon nanotube (CNT) was prepared. The presence of PNIPAM shell on cellulose nanofibrils (CNFs) endow the composite membrane with thermal responsiveness. By external stimulation, an increase temperature from 10 °C to 70 °C allows the average pore size of the membrane to be controlled from 28 nm to 110 nm, as well as the water permeance from 440 L·m−2·h−1·bar−1 to 1088 L·m−2·h−1·bar−1. The gating ratio of the membrane can reach 2.47. The photothermal effect of CNT rapidly warms up the membrane to the lowest critical solution temperature in the water, avoiding the constraint that the whole water phase cannot be heated throughout the practical use process. The membrane can precisely control the nanoparticles to concentrate at 25.3 nm, 47.7 nm or 102 nm by adjust the temperature. In addition, the water permeance can be restored to 370 L·m−2·h−1·bar−1 by washing the membrane under light. The smart gating membrane has a wide application in substance multi-stage separation and selective separation, and it can realize self-cleaning.

A Thermo-Responsive Polymer Micelle with a Liquid Crystalline Core.

An amphiphilic diblock copolymer (PChM-PNIPAM), composed of poly(cholesteryl 6-methacryloyloxy hexanoate) (PChM) and poly(N-isopropyl acrylamide) (PNIPAM) blocks, was prepared via reversible addition-fragmentation chain transfer radical polymerization. The PChM and PNIPAM blocks exhibited liquid crystalline behavior and a lower critical solution temperature (LCST), respectively. PChM-PNIPAM formed water-soluble polymer micelles in water below the LCST because of hydrophobic interactions of the PChM blocks. The PChM and PNIPAM blocks formed the core and hydrophilic shell of the micelles, respectively. With increasing temperature, the molecular motion of the pendant cholesteryl groups increased, and a liquid crystalline phase transition occurred from an amorphous state in the core. With further increases in temperature, the PNIPAM block in the shell exhibited the LCST and dehydrated. Hydrophobic interactions of the PNIPAM shells resulted in inter-micellar aggregation above the LCST.

Magnetic Field-Assisted Fast Assembly of Microgel Colloidal Crystals.

Compared with the colloidal crystals (CCs) of hard spheres, large-scale, high-quality CCs of soft microgel spheres are easier to be assembled because they are more tolerant to defects. However, to assemble microgel CCs, a microgel dispersion should first be concentrated and then allowed to crystallize, which is tedious and time-consuming. Herein, we demonstrated that a magnetic poly(N-isopropylacrylamide) (PNIPAM) microgel with an Fe3O4 core and a PNIPAM shell can be assembled into CCs quickly by simply applying an external magnetic field to the diluted microgel dispersions. The resulting CCs are highly ordered as revealed by their iridescent color, laser diffraction pattern, and confocal characterization. They display a sharp Bragg peak on their reflection spectra, which shifts to lower wavelength when heated because of the thermosensitivity of the PNIPAM shell. The magnetic assembly is not only simple and fast but also allows control of the CC structure in both horizontal and vertical directions. Using spatially varying magnetic fields, patterned microgel CCs were facilely assembled. More importantly, magnetic microgel spheres with different sizes can be assembled in a layer-by-layer manner by adding them sequentially, and the thickness of each layer can be simply controlled by the amount of spheres added.

Thermosensitive Core-Shell Fe3O4@poly(N-isopropylacrylamide) Nanogels for Enhanced Oil Recovery.

An investigation on the application of thermosensitive core-shell Fe3O4@PNIPAM nanogels in enhanced oil recovery was successfully performed. Here, the unique core-shell architecture was fabricated by conducting the polymerization at the surface of 3-butenoic acid-functionalized Fe3O4 nanoparticles and characterized using X-ray diffraction (XRD), 1H NMR, vibration sample magnetometer (VSM), and high-resolution transmission electron microscopy (HR-TEM). According to the results, this core-shell structure was beneficial for achieving the desired high viscosity and low nanofluid mobility ratio at high temperatures, which is essential for enhanced oil recovery (EOR) application. The results demonstrated that the nanogels exhibited a unique temperature-dependent flow behavior due to the PNIPAM shell's ability to transform from a hydrated to a dehydrated state above its low critical solution temperature (LCST). At such conditions, the nanogels exhibited a significantly low mobility ratio (M = 0.86), resulting in an even displacement front during EOR and leads to higher oil production. Based on the result obtained from sand pack flooding, about 25.75% of an additional secondary oil recovery could be produced when the nanofluid was injected at a temperature of 45 °C. However, a further increase in the flooding temperature could result in a slight reduction in oil recovery due to the precipitation of some of the severely aggregated nanogels at high temperatures.

Self-Assembled Micelles from Thermoresponsive Poly(methyl methacrylate)-b-poly(N-isopropylacrylamide) Diblock Copolymers in Aqueous Solution

The temperature-dependent phase behavior and self-assembly behavior in aqueous solution of the thermoresponsive amphiphilic diblock copolymer PMMA21-b-PNIPAM283 made of a short permanently hydrophobic poly(methyl methacrylate) block and a long thermoresponsive poly(N-isopropylacrylamide) are studied. Turbidimetry, dynamic light scattering (DLS), and synchrotron small-angle X-ray scattering (SAXS) provide temperature-dependent structure information. A lower critical solution temperature (LCST) behavior with a cloud point TCP = 31.1 °C in dilute solution is observed. Below TCP, spherical core–shell micelles are present, having a small PMMA core and a hydrated PNIPAM shell with a radial gradient of water content. Below TCP, the micelles are interpenetrated and show a weak correlation with each other. As the temperature approaches TCP, the micellar core shrinks and thus, the aggregation number decreases, revealing that the PMMA blocks are still mobile. Moreover, the micellar shell dehydrates above TCP and the micelles notably contract. They form clusters, which grow and transform into large compact aggregates as temperature is raised far above TCP.

Preparation, self-assembly of SiO2/PNIPAm complex microgels and their manipulation of fluorescence emission for organic dyes

In this study, a novel strategy for manipulating fluorescence emission of organic dyes is reported, which is based on coupling optical properties of colloidal crystals (CCs) with responsive microgels. Firstly, SiO2 microspheres doped with three kinds of organic dyes (Rhodamine B, RhB; fluorescein isothiocyanate, FITC; commercial cationic Fluorescent Yellow, X-10GFF) were prepared and they were used as the cores to synthesize SiO2/PNIPAm complex microgels doped with organic dyes by free radical polymerization. Then 3D self-assembled CCs of the complex microgels were fabricated by centrifugation. The microstructure of the complex microgel was characterized by Fourier transform infrared (FTIR), transmission electron microscopy (TEM), thermogravimetric (TG), dynamic light scattering (DLS), and differential scanning calorimeter (DSC). Moreover, the effect of doping organic dyes and temperature on self-assembly of the microgels were investigated. Manipulation of fluorescence emission for organic dyes by CCs was studied by photoluminescence (PL) and UV-visible spectrophotometer (UV-Vis). The results indicate that, due to the soft and thermosensitive property of PNIPAm shell, continuous adjustment to the photonic bandgap (PBG) of the CCs can be achieved conveniently by varying concentrations of the complex microgels or ambient temperatures, and when PBG of the CCs overlaps with the fluorescence emission peak of the organic dye, fluorescence emission of the organic dye can be manipulated.

Synthesis and structure of temperature-sensitive nanocapsules

The transport and systematic release of functional agents at specific areas are key challenges in various application fields. These make the development of micro- and nanocapsules, which allow for uptake, storage, and triggered release, of high interest. Hollow thermoresponsive microgels, cross-linked polymer networks with a solvent-filled cavity in their center, are promising candidates as triggerable nanocapsules, as they can adapt their size and shape to the environment. Their shell permeability can be controlled by temperature, while the cavity can serve as a storage place for guest species. Here, we present the synthesis and structural characterization of temperature-responsive microgels, which are deswollen at room temperature and swell upon moderate cooling, to facilitate potential encapsulation experiments. We present microgels made from poly(N-isopropylacrylamide-co-diacetone acrylamide), p(NIPAM-co-DAAM), possessing a volume phase transition temperature below room temperature. Their colloidal stability in the deswollen state can be enhanced by adding a swollen polymer shell made of poly(N-isopropylacrylamide), pNIPAM, as periphery. The synthesis of hollow double-shell microgels comprising a cavity surrounded by an inner p(NIPAM-co-DAAM) shell and an outer pNIPAM shell is established. The inner network enables the control of the shell permeability: the network is deswollen at room temperature and swells upon moderate cooling. The outer network guarantees for steric stability at room temperature. Light scattering techniques are employed for the characterization of the microgels. Form factor analysis reveals that the cavity of the nanocapsules persists at all swelling states, making it an ideal site for the storage of guest species.

Stopped-Flow Dynamics Study on the Escape Behavior of Polyelectrolyte Macromolecules from Microgels: The Influence of the Path Length and Size.

We reported the fabrication of several monodispersed poly(2-vinyl pyridine)-poly(N-isopropylacrylamide) (P2VP-PNIPAM) microgels including the P2VP core (non-cross-linked) and PNIPAM (cross-linked) shell by mature emulsion polymerization. The fast escape behavior (diffusion process) of linear P2VP chains through a porous PNIPAM layer was investigated by a pH jump stopped-flow apparatus. The time-dependent dynamic traces (corresponding to the scattered light intensity) decreased at the initial timescale of several seconds and then reached an apparent equilibrium, confirming the efficient escape of P2VP chains from microgels. Compared with the previously reported literature, such an accelerated escape process resulted from the sharply increased internal charge repulsive force caused by the protonation of P2VP moieties under acidic conditions. The obtained characteristic relaxation times by single exponential fitting of these kinetic traces were dependent on the final pH values, equilibrium temperatures, shell thickness (path length), and cross-linking density (mesh size). We believe that this work can provide an efficient way to investigate hindered diffusion, especially the initial rapid diffusion stage. Not only that, the proposed model can also provide theoretical guidance to some practical applications, such as membrane separation and the exocytosis phenomenon of intracellular proteins or macromolecular substances.

Dual-emission hydrogel nanoparticles with linear and reversible luminescence-response to pH for intracellular fluorescent probes

A type of dual-emission probe with highly recognizable luminescence-response to pH has been designed. For the prepared core-shell polymeric hydrogel nanoparticles probe (Eu(DBM)3Phen doped polystyrene (PS)-co-poly(N-isopropylacrylamide)(PNIPAM)/FITC), the red emission of inner encapsulated europium complexes Eu(DBM)3Phen is remained in the hydrophobic PS core and used as a stable reference signal. Comparingly, the green emission of outer electrostatic bonded fluorescent isothiocyanate (FITC) moieties on the hydrophilic PNIPAM shell is adjusted and acted linear and reversible luminescence-response to pH between 5.8 and 7.4 with an exact resolution of 0.1 units. As a remarkable and smart pH probe, the hydrogel nanoparticles show low biological toxicity and prolonged resistance to ions and photobleaching. Also, the probes have successfully discriminated the fluorescent imaging for cytoplasmic matrix based on different pH with minimum biologic background fluorescence. These dual-emission pH-sensitive hydrogel nanoparticles suggest potential applications in clinical medicine, such as cell imaging and disease diagnosis.

Stimuli-responsive microgels for controlled deposition of gold nanoparticles on surfaces.

A variety of gold nanoparticle (AuNP) core/poly(N-isopropylacrylamide) (pNIPAm) shell microgels (Au@pNIPAm) were generated using seed-mediated polymerization. The shell thickness and AuNP core diameter were easily tunable at the time of synthesis. The resultant Au@pNIPAm microgels were characterized via photon-correlation spectroscopy, transmission electron microscopy and ultraviolet-visible spectroscopy. AuNP arrays were generated by “painting” the microgels on a surface, using the shell thickness to define the distance between the AuNPs, followed by shell removal via plasma etching. We found that when the pNIPAm shell thickness decreased (via its tuning at the time of synthesis or deposition at elevated temperature at which the shell is collapsed) the AuNPs were closer to one another. We also showed that via sequential deposition Au@pNIPAm microgels with different AuNP core sizes could be deposited on a single surface. The presented “painting protocol” offers a facile way to coat large area surfaces quickly which is not easily achievable using other approaches. We envision that this approach is extremely versatile, allowing a number of different nanomaterials embedded in pNIPAm shells to be deposited/patterned on surfaces. With the control over the deposition on the surface that we show here, we hope that the Au@pNIPAm microgels will find use in lithography/surface patterning applications.

Triple-Responsive Pickering Emulsion Stabilized by Core Cross-linked Supramolecular Polymer Particles.

It is significant to explore multiresponsive Pickering emulsions because of their flexibility in terms of demulsification in comparison with the single stimuli-responsive systems. In this study, we described a triple-responsive oil-in-water Pickering emulsion that was stabilized by amphiphilic core cross-linked supramolecular polymer particles (CCSPs). For this purpose, β-cyclodextrin-terminated poly(N-isopropylacrylamide) (PNIPAM-β-CD) and azobenzene-capped poly(4-vinylpyridine) (P4VP-azo) were separately synthesized by reversible addition-fragmentation chain transfer polymerization. By virtue of the inclusion interaction between the β-CD host and the azobenzene guest in dimethyl sulfoxide, the amphiphilic supramolecular block copolymer, poly(4-vinylpyridine)-b-poly(N-isopropylacrylamide) (P4VP-b-PNIPAM), was formed. CCSPs were prepared through the combination of the self-assembly of P4VP-b-PNIPAM in the selective solvent, water, and the cross-linking of the P4VP core with 1,4-dibromobutane. Due to thermoresponsiveness of PNIPAM shells and the supramolecular linkages between the cross-linked hydrophobic P4VP core and hydrophilic PNIPAM shells, the as-prepared CCSPs exhibited temperature-, light-, and amantadine hydrochloride guest-triggered morphological transitions. Such triple-responsive morphological transitions gifted CCSPs stabilized oil-in-water Pickering emulsion with flexible demulsification in response to various factors, such as thermo, light, and amantadine hydrochloride or their combinations. Such triple-responsive oil-in-water Pickering emulsion also provided an ideal platform for heterogeneous reactions conducted at the oil-water interface. A large interfacial area and responsive demulsification allowed the reaction to be performed with an efficient and sustainable pattern.

Motile Artificial Chromatophores: Light‐Triggered Nanoparticles for Microdroplet Locomotion and Color Change

AbstractGold nanoparticles coated with a poly(N‐isopropylacrylamide) (pNIPAM) shell undergo reversible dis/assembly below and above the critical temperature of 32 °C. Loading these particles into microdroplets at high density creates light‐driven artificial chromatophores. Triggering the nanoparticle assembly gives dramatic color changes from nanoparticle localization at the base of the droplets, resembling zebrafish melanophores. These reversible chromatophore states can be switched by both bulk and optical heating, explored here in individual microdroplets and in large cm2 areas of close‐packed droplets. Illuminating chromatophores off‐center with a tightly focused beam results in droplet locomotion via two separate mechanisms, Marangoni interfacial shear and gas bubble propulsion, depending on optical power.

Temperature–Light Dual‐Responsive Au@PNIPAm Core‐Shell Microgel‐Based Optical Devices

AbstractAu nanoparticle (AuNP) core particles coated with a poly(N‐isopropylacrylamide) (pNIPAm) shell (Au@pNIPAm) are synthesized by seed mediated free radical polymerization. Subsequently, a temperature–light‐responsive photonic device is fabricated by sandwiching the Au@pNIPAm particles between two thin layers of Au. The optical device exhibits visual color and characteristic multipeak reflectance spectra, where peak position is primarily determined by the distance between two Au layers. Dual responsivities of the photonic device are achieved by combining the photothermal effect of AuNPs core (localized surface plasmon resonance (LSPR) effect) and the temperature responsivity of the pNIPAm shell. That is, the pNIPAm shell collapses as the temperature is increased above pNIPAm's lower critical solution temperature, either by direct heat input or heat generated by AuNPs' LSPR effect. To investigate the effect of AuNPs distribution in the microgels on the devices' photothermal responsivity, the Au@pNIPAm microgel‐based etalon devices are compared with that fabricated by AuNP‐doped pNIPAm‐based microgels; in terms of response kinetics and optical spectrum homogeneity. The uniform Au@pNIPAm microgel‐based devices show a fast response and exhibit a comparatively homogeneous spectrum over the whole slide. These materials can potentially find use in drug delivery systems, active optics, and soft robotics.

Bioinspired dual stimuli-responsive membranes with enhanced gating ratios and reversible performances for water gating

Self-regulation of membrane permeability performance is highly desirable for porous membrane applications. Inspired by the stomatal closure behaviour of plant leaves in response to environmental changes, here we report a series of dual thermo- and pH-responsive membranes based on the poly(4-vinyl pyridine) (P4VP) core/poly(N-isopropylacrylaminde) (PNIPAM) shell microgels. The stimuli-responsive microgels underwent in situ surface segregation and uniformly decorated on the surface of internal channels during the phase inversion process. The hydraulic permeability performance of the dual responsive membranes (DRMs) has been investigated within a temperature range of 20–50 °C and a wide pH range (spanning pH 2–6). The water flux of optimized membrane (M2) varied from 1.94 kg m−2 h−1 at 20 °C/pH 2–474.91 kg m−2 h−1 at 50 °C/pH 6 with a high gating ratio of 245. Investigations revealed that microgels based on different thickness of PNIPAM shell conferred different thermo-/pH-responsive properties to the DRMs. For example, the thicker PNIPAM shell enhanced the thermo-response performance, while the pH-response performance was restrained. These optimum smart gating membranes with enhanced gating coefficient and reversibility are potential for the applications in water gating and controlled release systems.

Probing the Internal Heterogeneity of Responsive Microgels Adsorbed to an Interface by a Sharp SFM Tip: Comparing Core-Shell and Hollow Microgels.

Microgels composed of thermoresponsive polymer poly( N-isopropylacrylamide) (PNIPAM) are interfacial active. Their adsorption leads to deformation, causing conformational changes that have profound effects on the macroscopic properties of these films. Yet, methods to quantitatively probe the local density are lacking. We introduced scanning force microscopy (SFM) to quantitatively probe the internal structure of microgels physically adsorbed on a solid (SiO2)/water interface. Using a sharp SFM tip, we investigated the two types of microgels: (i) core-shell microgels featuring a hard silica core and a PNIPAM shell and (ii) hollow microgels obtained by dissolution of the silica core. Thus, both systems have the same polymer network as the peripheral structure but a distinctly different internal structure, that is, a rigid core versus a void. By evaluating the force-distance curves, the force profile during insertion of the tip into the polymer network enables to determine a depth-dependent contact resistance, which closely correlates with the density profiles determined in solution by small-angle neutron scattering. We found that the cavity of the swollen hollow microgels is still present when adsorbed to the solid substrate. Remarkably, while currently used techniques such as colloidal probe or reflectometry only provide an average of the z-profile, the methodology introduced herein actually probes the real three-dimensional density profile, which is ultimately important to understand the macroscopic behavior of microgel films. This will bridge the gap between the colloidal probe experiments that deform the microgel globally and the insertion in which the disturbance is located near the tip.

Emulsions stabilized by pH-responsive PNIPAM-based microgels: Effect of spatial distribution of functional carboxylic groups on the emulsion stability

Abstract Poly(N-isopropylacrylamide-co-Methacrylic acid) (PNIPAM-MAA) microgels with different spatial distribution of functional carboxylic (COOH) groups were synthesized by a combination of semi-batch and temperature-programmed surfactant-free precipitation polymerization. This synthetic approach enabled functional COOH groups and crosslinks to be controlled in a better way so that they were either predominately concentrated at the periphery, leading to a functional dense-shell (DS), or mainly located inside the microgel, resulting in a functional dense-core (DC) particle. Because of the specially designed internal structures of these two microgels, we were able to investigate the effect of the charge group distribution on the corresponding Pickering emulsions. By examining the emulsion stability at different pH values and particle concentration using these two microgel samples as particular emulsifiers, our results showed that the soft, negatively charged microgel with a pure PNIPAM shell is the best emulsion stabilizer since the microgel is very hydrophilic and also retains its interfacial activity at the same time. On the other hand, the functional DS microgel lost most of its interfacial activity due to the dramatic increase in hydrophilicity, particularly in alkaline condition. Nevertheless, it is still capable of stabilizing oil/water emulsion by its high volume fraction in the continuous phase. Although the particles are not strongly adsorbed to the interface, the movement of the particles is significantly restrained. Therefore, they are still separating the oil droplets from coalescence.

Thermally Tunable Pickering Emulsions Stabilized by Carbon-Dot-Incorporated Core-Shell Nanospheres with Fluorescence "On-Off" Behavior.

Lack of deep understanding of nanoparticle (NP) actions at oil/water interface set an obstacle to practical applications of Pickering emulsions. Fluorescence labels fabricated by incorporation of carbon dots (CDs) into poly(N-isopropylacrylamide) (PNIPAM) matrix can not only mark the action of PNIPAM-based NPs in the interface but also reflect the colloidal morphologies of PNIPAM. In this work, we employed coaxial electrospraying for fabricating core-shell nanospheres of cellulose acetate encapsulated by PNIPAM, and facile incorporation of CDs in PNIPAM shells was achieved simultaneously. The coaxial electrosprayed NPs (CENPs) with temperature-dependent wettability can stabilize heptane and toluene in water at 25 °C, respectively, and reversible emulsion break can be triggered by temperature adjustment around the low critical solution temperature (LCST). Remarkably, CENP/CD composites exhibited a fluorescence "on-off" behavior because of the volume phase transition of the PNIPAM shell. CENP/CD composites in Pickering emulsions clearly elucidated the motions of CENPs in response to temperature changes. At temperatures below the LCST, the CENP concentration played an important role in surface coverage of oil droplets. Specifically, the CENP concentration above the minimum concentration for complete emulsification of oil phase led to high surface coverage and two-domain adsorption of CENPs at the interface including primary monolayer anchoring of CENPs on droplets surrounded by interconnected CENP networks, which contributed to the superior stability of the emulsions. Moreover, CENP/CD composites can be recycled with well-preserved core-shell structure and stable fluorescent properties, which offers their great potential applications in sensors and imaging.