Gene/Protein Disease Symptom Drug Enzyme Compound
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Two novel double hydrophilic multiblock copolymers of N,N-dimethylacrylamide and N-isopropylacrylamide, m-PDMAp-PNIPAMq, with varying degrees of polymerization (DPs) for PDMA and PNIPAM sequences (p and q) were synthesized via consecutive reversible addition-fragmentation chain transfer (RAFT) polymerizations using polytrithiocarbonate (1) as the chain transfer agent (Scheme 1), where PDMA is poly(N,N-dimethylacrylamide) and PNIPAM is poly(N-isopropylacrylamide). The DPs of PDMA and PNIPAM sequences were determined by 1H NMR, and the block numbers, i.e., number of PDMAp-PNIPAMq sequences (n), were obtained by comparing the molecular weights of multiblock copolymers to that of cleaved products as determined by gel permeation chromatography (GPC). m-PDMA42-PNIPAM37 and m-PDMA105-PNIPAM106 multiblock copolymers possess number-average molecular weights (Mn) of 4.62x10(4) and 9.53x10(4), respectively, and the polydispersities (Mw/Mn) are typically around 1.5. Block numbers of the obtained multiblock copolymers are ca. 4, which are considerably lower than the numbers of trithiocarbonate moieties per chain of 1 (approximately 20) and m-PDMAp precursors (approximately 6-7). PDMA homopolymer is water soluble to 100 degrees C, while PNIPAM has been well known to exhibit a lower critical solution temperature (LCST) at ca. 32 degrees C. In aqueous solution, m-PDMA42-PNIPAM37 and m-PDMA105-PNIPAM106 multiblock copolymers molecularly dissolve at room temperature, and their thermo-induced collapse and aggregation properties were characterized in detail by a combination of optical transmittance, fluorescence probe measurements, laser light scattering (LLS), and micro-differential scanning calorimetry (micro-DSC). It was found that chain lengths of PDMA and PNIPAM sequences exert dramatic effects on their aggregation behavior. m-PDMA105-PNIPAM106 multiblock copolymer behaves as protein-like polymers and exhibits intramolecular collapse upon heating, forming unimolecular flower-like micelles above the thermal phase transition temperature. On the other hand, m-PDMA42-PNIPAM37 multiblock copolymer exhibits collapse and intermolecular aggregation, forming associated multimolecular micelles at elevated temperatures. The intriguing aggregation behavior of this novel type of double hydrophilic multiblock copolymers argues well for their potential applications in many fields such as biomaterials and biomedicines.
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PMID:Thermo-induced formation of unimolecular and multimolecular micelles from novel double hydrophilic multiblock copolymers of N,N-dimethylacrylamide and N-isopropylacrylamide. 1802 77

A novel thermo- and pH-sensitive nanogel particle, which is a core-shell structured particle with a poly(N-isopropylacrylamide) (p(NIPAAm)) hydrogel core and a poly(ethylene glycol) monomethacrylate grafted poly(methacrylic acid) (p(MMA-g-EG)) shell, is of interest as a vehicle for the controlled release of peptide drugs. The interactions between such nanogel particles and artificial mucin layers during both approach and separation were successfully measured by using colloid probe atomic force microscopy (AFM) under various compression forces, scan velocities, and pH values. While the magnitudes of the compression forces and scan velocities did not affect the interactions during the approach process, the adhesive force during the separation process increased with these parameters. The pH values significantly influenced the interactions between the nanogel particles and a mucin layer. A large steric repulsive force and a long-range adhesive force were measured at neutral pH due to the swollen p(MMA-g-EG) shell. On the other hand, at low pH values, the steric repulsive force disappeared and a short-range adhesive force was detected, which resulted from the collapse of the shell layer. The nanogel particles possessed a pH response that was sufficient to protect the incorporated peptide drug under the harsh acidic conditions in the stomach and to effectively adhere to the mucin layer of the small intestine, where the pH is neutral. The relationships among the nanogel particle-mucin layer interactions, pH conditions, scan velocities, and compression forces were systemically investigated and discussed.
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PMID:Direct measurement of interactions between stimulation-responsive drug delivery vehicles and artificial mucin layers by colloid probe atomic force microscopy. 1831 15

We describe a magnetic nanoparticle drug carrier for controlled drug release that responds to the change in external temperature or pH, with characteristics of longer circulation time and reduced side effects. The novel nanocarrier is characterized by a functionalized magnetite (Fe(3)O(4)) core that is conjugated with drug via acid-labile hydrazone-bond and encapsulated by the thermosensitive smart polymer, chitosan-g-poly(N-isopropylacrylamide-co-N,N-dimethylacrylamide) [chitosan-g-poly(NIPAAm-co-DMAAm)]. The chitosan-g-poly(NIPAAm-co-DMAAm) smart polymer exhibits a lower critical solution temperature (LCST) of approximately 38 degrees C, signifying phase transition behavior of the smart polymer and enabling its use for triggering on-off mechanisms. The drug release response was appreciably low at a temperature less than the LCST as compared with a temperature above the LCST. In each case, there was an initial rapid drug release, followed by a controlled released in the second stage, especially in a mild acidic buffer solution of pH 5.3. We believe that the drug release occurs via a collapse of the encapsulated thermosensitive polymer and cleavage of the acid-labile hydrazone linkage.
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PMID:A stimulus-responsive magnetic nanoparticle drug carrier: magnetite encapsulated by chitosan-grafted-copolymer. 1832 48

Synthetic polycations have shown promise as gene delivery vehicles but suffer from an unacceptable toxicity and low transfection efficiency. Novel architectures are being explored to increase transfection efficiency, including copolymers with a thermoresponsive character. The physicochemical characterization of a family of copolymers comprising a core of the cationic polymer poly(ethylene imine) (PEI) with differing thermoresponsive poly( N-isopropylacrylamide) (PNIPAM) grafts has been carried out using pulsed-gradient spin-echo NMR (PGSE-NMR) and small-angle neutron scattering (SANS). For the copolymers that have longer chain PNIPAM grafts, there is clear evidence of the collapse of the grafts with increasing temperature and the associated emergence of an attractive interpolymer interaction. These facets depend on the number of PNIPAM grafts attached to the PEI core. While a collapse in the smaller PNIPAM grafts is observed for the third polymer, there is no appearance of the interpolymer attractive interaction. These observations provide further insight into the association behavior of these copolymers, which is fundamental to developing a full understanding of how they interact with nucleic acids. Furthermore, the differing behaviors of the three copolymers over temperatures in which the PNIPAM blocks undergo coil-to-globule transitions is indicative of changes in the presentation of charged-core and hydrophobic chain components, which are key factors affecting nucleic acid binding and, ultimately, cell transfection ability.
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PMID:Physicochemical characterization of thermoresponsive poly(N-isopropylacrylamide)-poly(ethylene imine) graft copolymers. 1834 32

Smart thermoresponsive gels and cryogels with incorporated emulsions have been synthesized and studied. The gels were obtained by three-dimensional copolymerization of N-isopropylacrylamide and N,N'-methylene-bis-acrylamide or N,N'-bis(acryloyl)cystamine in the presence of dispersion of tetradecane stabilized with sodium dodecylsulfate. Polymerization was performed at room temperature and below the water crystallization temperature. Both composite gels and cryogels were capable of heat-induced collapse. The extent of the collapse of the composite gel prepared at room temperature was much smaller and without squeezing of the lipophilic phase out of the shrunk composite gel. In contrast, shrinking of the composite cryogel was accompanied by release of tetradecane emulsion.
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PMID:Intelligent gels and cryogels with entrapped emulsions. 1838 80

We describe the synthesis, characterisation and surface-modification of magnetic nanoparticles and a poly(N-isopropylacrylamide) microgel, followed by the assembly and characterisation of magnetic nanoparticles on the microgel. To facilitate this deposition, the surface of the microgel is first modified via the layer-by-layer assembly of polyelectrolytes. One advantage of this concept is that it allows an independent optimization and fine tuning of the magnetic and thermoresponsive properties of individual components (nanoparticles and microgels) before assembling them so that the hybrid core-shell structure retains all the individual properties. The decisive parameter when exploiting the thermoresponsive and magnetic properties in such hybrid core-shell structures is the amount of heat transfer from the magnetic core onto the thermosensitive (loaded) microgel (for the subsequent heat-triggered release of drugs). Inductive heat study reveals that the heat generated by the magnetic nanoparticles is sufficient to cause the collapse of the microgel above its volume phase transition temperature. Successful confinement of positively and negatively charged magnetic nanoparticles between polyelectrolyte layers is achieved using the layer-by-layer deposition onto the microgel. Dynamic light scattering measurements show (i) the presence of each layer successfully deposited, (ii) the preservation of thermoresponsivity in the coated microgel, and (iii) that the magnetic nanoparticles do not get detached during the phase transition of the microgel. Electrophoresis measurements confirm charge reversal at every stage of layering of polycations, polyanions and magnetic nanoparticles. This unique combination of thermoresponsivity and magnetism opens up novel perspectives towards remotely controlled drug carriers.
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PMID:Dual-stimuli responsive PNiPAM microgel achieved via layer-by-layer assembly: magnetic and thermoresponsive. 1851 12

This paper deals with a thermo-responsive poly(N-isopropylacrylamide) (NIPA) gel containing a polymeric surfactant poly(2-(methacryloyloxyl)decylphosphate) (PMDP) which shows rapid volume change above phase transition temperature at ca. 34 degrees C. Based on the measurements of dye-solubilization, it was suggested that intra-molecular micelles of the polymeric surfactant PMDP are inside NIPA gel-network. It is concluded that the intra-molecular micelles of polymeric surfactant involving NIPA chains may play crucial role in the rapid collapse of the NIPA-PMDP gel at the phase transition temperature.
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PMID:Thermo-responsive poly(N-isopropylacrylamide) gel containing polymeric surfactant poly(2-(methacryloyloxyl)decylphosphate): correlation between rapid collapsing characters and micelles of polymeric surfactant. 1853 10

Poly(N-isopropylmethacrylamide) (PiPMA) has one more methyl group at each monomeric unit than poly(N-isopropylacrylamide) (PiPA). By use of laser light scattering (LLS) and ultrasensitive differential scanning calorimetry (US-DSC) we have investigated the association and dissociation of PiPMA chains in water. LLS studies reveal that PiPMA chains form larger aggregates at a temperature above its lower critical solution temperature (LCST) as the chain molar mass (Mw) decreases. In comparison with PiPA aggregates, PiPMA aggregates show a larger ratio of average radius of gyration to average hydrodynamic radius (<Rg>/<Rh>), indicating that PiPMA aggregates are looser. US-DSC studies show PiPMA chains have smaller enthalpy change (DeltaH) and entropy change (DeltaS) than PiPA chains during the phase transition, indicating that PiPMA chains have smaller conformational change. Our experiments demonstrate that the additional methyl groups in PiPMA chains restrain the intrachain collapse and interchain association, leading the phase transition to occur at a higher temperature.
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PMID:Role of methyl in the phase transition of poly(N-isopropylmethacrylamide). 1858 6

The effects of the concentration (C) and heating rate on the collapse and association of poly(N-isopropylacrylamide) chains in water have been investigated by use of ultrasensitive differential scanning calorimetry. In the dilute solutions, both the phase transition temperature (Tp) and enthalpy change (DeltaH) increase with the heating rate but decrease with concentration. By extrapolation to zero heating rate and zero concentration, Tp and DeltaH for coil-to-globule transition of a single chain in thermodynamic equilibrium can be obtained. In semidilute solutions, both Tp and DeltaH increase with the heating rate but slightly vary with the concentration. Tp and DeltaH for pure interchain association in equilibrium are obtained by extrapolation to zero heating rate. Our experiments reveal that only intrachain contraction occurs when the concentration is infinitely close to zero. When the concentration is above the overlap concentration (C*), only interchain association exists. In the range 0<C<C*, both intrachain contraction and interchain association coexist.
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PMID:Can coil-to-globule transition of a single chain be treated as a phase transition? 1858 31

Hydrogel nanocomposites are novel macromolecular biomaterials that promise to impact various applications in medical and pharmaceutical fields. In this paper, magnetic nanocomposites of temperature responsive hydrogels were used to illustrate remote controlled (RC) drug delivery. A high frequency alternating magnetic field (AMF) was used to trigger the on-demand pulsatile drug release from the nanocomposites. Nanocomposites were synthesized by incorporation of superparamagnetic Fe(3)O(4) particles in negative temperature sensitive poly (N-isopropylacrylamide) hydrogels. Pulses of AMF were applied to the nanocomposites and the kinetics of collapse and recovery were characterized. Application of AMF resulted in uniform heating within the nanocomposites leading to accelerated collapse and squeezing out large amounts of imbibed drug (release at a faster rate). Remote controlled pulsatile drug release was characterized for different drugs as well as for different ON-OFF durations of the AMF.
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PMID:Magnetic hydrogel nanocomposites for remote controlled pulsatile drug release. 1860 1


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