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Herein, we report a stimuli-responsive hydrogel with inhibitory activity against Escherichia coli prepared by chemical crosslinking of carboxymethyl chitosan (CMCs) and hydroxyethyl cellulose (HEC). The hydrogels were prepared by esterification of chitosan (Cs) with monochloroacetic acid to produce CMCs which were then chemically crosslinked to HEC using citric acid as the crosslinking agent. To impart a stimuli responsiveness property to the hydrogels, polydiacetylene-zinc oxide (PDA-ZnO) nanosheets were synthesized in situ during the crosslinking reaction followed by photopolymerization of the resultant composite. To achieve this, ZnO was anchored on carboxylic groups in 10,12-pentacosadiynoic acid (PCDA) layers to restrict the movement of the alkyl portion of PCDA during crosslinking CMCs and HEC hydrogels. This was followed by irradiating the composite with UV radiation to photopolymerize the PCDA to PDA within the hydrogel matrix so as to impart thermal and pH responsiveness to the hydrogel. From the results obtained, the prepared hydrogel had a pH-dependent swelling capacity as it absorbed more water in acidic media as compared to basic media. The incorporation of PDA-ZnO resulted in a thermochromic composite responsive to pH evidenced by a visible colour transition from pale purple to pale pink. Upon swelling, PDA-ZnO-CMCs-HEC hydrogels had significant inhibitory activity against E. coli attributed to the slow release of the ZnO nanoparticles as compared to CMCs-HEC hydrogels. In conclusion, the developed hydrogel was found to have stimuli-responsive properties and inhibitory activity against E. coli attributed to zinc nanoparticles.

Due to their highly hydrophilic nature and compositional versatility, hydrogels have assumed a protagonic role in the development of physiologically relevant tissues for several biomedical applications, such as in vivo tissue replacement or regeneration and in vitro disease modeling. By forming interconnected polymeric networks, hydrogels can be loaded with therapeutic agents, small molecules, or cells to deliver them locally to specific tissues or act as scaffolds for hosting cellular development. Hydrogels derived from decellularized extracellular matrices (dECMs), in particular, have gained significant attention in the fields of tissue engineering and regenerative medicine due to their inherently high biomimetic capabilities and endowment of a wide variety of bioactive cues capable of directing cellular behavior. However, these hydrogels often exhibit poor mechanical stability, and their biological properties alone are not enough to direct the development of tissue constructs with functional phenotypes. This review highlights the different ways in which external stimuli (e.g., light, thermal, mechanical, electric, magnetic, and acoustic) have been employed to improve the performance of dECM-based hydrogels for tissue engineering and regenerative medicine applications. Specifically, we outline how these stimuli have been implemented to improve their mechanical stability, tune their microarchitectural characteristics, facilitate tissue morphogenesis and enable precise control of drug release profiles. The strategic coupling of the bioactive features of dECM-based hydrogels with these stimulation schemes grants considerable advances in the development of functional hydrogels for a wide variety of applications within these fields.

Polypeptoids have attracted a lot of atteSDntion because of their unique structural characteristics and special properties. Polypeptoids have the same main chain structures to polypeptides, making them have low cytotoxicity and excellent biocompatibility. Polypeptoids can also respond to external environmental changes by modifying the configurations of the side chains. The external stimuli can be heat, pH, ions, ultraviolet/visible light and active oxygen or their combinations. This review paper discussed the recent research progress in the field of stimulus-responsive polypeptoids, including the design of new stimulus-responsive polypeptoid structures, controlled actuation factors in response to external stimuli and the application of responsive polypeptoid biomaterials in various biomedical and biological nanotechnology, such as drug delivery, tissue engineering and biosensing.

Intelligent materials, also known as smart materials, are capable of reacting to various external stimuli or environmental changes by rearranging their structure at a molecular level and adapting functionality accordingly. The initial concept of the intelligence of a material originated from the natural biological system, following the sensing–reacting–learning mechanism. The dynamic and adaptive nature, along with the immediate responsiveness, of the polymer- and fiber-based smart materials have increased their global demand in both academia and industry. In this manuscript, the most recent progress in smart materials with various features is reviewed with a focus on their applications in diverse fields. Moreover, their performance and working mechanisms, based on different physical, chemical and biological stimuli, such as temperature, electric and magnetic field, deformation, pH and enzymes, are summarized. Finally, the study is concluded by highlighting the existing challenges and future opportunities in the field of intelligent materials.

The temperature and mechanism of phase transition of poly(N-isopropylacrylamide-co-acrylic acid) [P(NiPAAm-co-AAc)], which is one of the multi-stimuli responsive polymers, were investigated at various pHs using infrared (IR) spectroscopy, two-dimensional (2D) gradient mapping, and two-dimensional correlation spectroscopy (2D-COS). The determined phase transition temperature of P(NiPAAm-co-AAc) at pH 4, 3, and 2 based on 2D gradient mapping and principal component analysis (PCA) showed that it decreases with decreasing pH, because COOH group in AAc changes with variation of pH. The results of 2D-COS analysis indicated that the phase transition mechanism of P(NiPAAm-co-AAc) hydrogel at pH4 is different from that at pH2 due to the effect of COOH group of AAc.

Eyesight is one of the most well-deserved blessings, amid all the five senses in the human body. It captures the raw signals from the outside world to create detailed visual images, granting the ability to witness and gain knowledge about the world. Eyes are exposed directly to the external environment; they are susceptible to the vicissitudes of diseases. The World Health Organization has predicted that the number of individuals affected by eye diseases will rise enormously in the next decades. However, the physical barriers of the eyes and the problems associated with conventional ocular formulations are significant challenges in ophthalmic drug development. This has generated the demand for a sustained ocular drug delivery system, which serves to deliver effective drug concentration at a reduced frequency for consistent therapeutic effect and better patient treatment adherence. Recent advancement in pharmaceutical dosage design has demonstrated that a stimuli-responsive in situ gel system exhibits the favorable characteristics for providing sustained ocular drug delivery and enhanced ocular bioavailability. Stimuli-responsive in situ gels undergo a phase transition (solution–gelation) in response to the ocular environmental temperature, pH, and ions. These stimuli transform the formulation into a gel at the cul de sac to overcome the shortcomings of conventional eye drops, such as rapid nasolacrimal drainage and short contact time with the ocular surface This review highlights the recent successful research outcomes of stimuli-responsive in situ gelling systems in treating in vivo models with glaucoma and various ocular infections. Additionally, it also presents the mechanism, recent development, and safety considerations of stimuli-sensitive in situ gel as the potential sustained ocular delivery system for treating common eye disorders.

In these times of Industrial 4.0 and Health 4.0, people currently want to enhance the ability of science and technology, to focus on patient aspects. However, with intelligent, green energy and biomedicine these days, traditional three-dimensional (3D) printing technology has been unable to meet our needs, so 4D printing has now arisen. In this research, a shape-memory composite material with 3D printing technology was used for 4D printing technology. The authors used fused deposition modeling (FDM) to print a polylactic acid (PLA) strip onto the surface of paper to create a shape-memory composite material, and a stimulus (heat) was used to deform and recover the shape of this material. The deformation angle and recovery angle of the material were studied with various processing parameters (heating temperature, heating time, pitch, and printing speed). This research discusses optimal processing related to shape-memory situations of stimulus-responsive composite materials. The optimal deformation angle (maximum) of the stimulus-responsive composite material was found with a thermal stimulus for an optimal heating temperature of 190 °C, a heating time of 20 s, a pitch of 1.5 mm, and a printing speed of 80 mm/s. The optimal recovery angle (minimum) of this material was found with a thermal stimulus for an optimal heating temperature of 170 °C, a heating time of 90 s, a pitch of 2.0 mm, and a printing speed of 80 mm/s. The most important factor affecting both the deformation and recovery angle of the stimulus-responsive composite material was the heating temperature. Refereed/Peer-reviewed

Injury to the central or peripheral nervous systems leads to the loss of cognitive and/or sensorimotor capabilities, which still lacks an effective treatment. Tissue engineering in the post-injury brain represents a promising option for cellular replacement and rescue, providing a cell scaffold for either transplanted or resident cells. Tissue engineering relies on scaffolds for supporting cell differentiation and growth with recent emphasis on stimuli responsive scaffolds, sometimes called smart scaffolds. One of the representatives of this material group is piezoelectric scaffolds, being able to generate electrical charges under mechanical stimulation, which creates a real prospect for using such scaffolds in non-invasive therapy of neural tissue. This paper summarizes the recent knowledge on piezoelectric materials used for tissue engineering, especially neural tissue engineering. The most used materials for tissue engineering strategies are reported together with the main achievements, challenges, and future needs for research and actual therapies. This review provides thus a compilation of the most relevant results and strategies and serves as a starting point for novel research pathways in the most relevant and challenging open questions.

In this work, a general, facile, and relatively low-cost method to produce electrically driven non-porous membranes by revalorization of recycled polyolefins is proposed. The polymer matrices are poly(propylene) (PP) and poly(ethylene) (PE) and their corresponding recycled samples, which are respectively mixed with carbon nanotubes (CNT). The performances of the elaborated nanocomposites are studied by morphological, rheological, and electrical conductivity tests. The Joule heating effect is evaluated by applying an electric field and recording the corresponding temperature rise. An increase of 90 &deg, C is obtained in certain cases, which represents the highest temperature enhancement reached so far by the Joule effect in thermoplastics, to our knowledge. The work shows a route to develop stimulus (voltage)-response (temperature) materials with low cost and with potential applications in many fields. As an example, the increase of the permeability with temperature of membranes made of the indicated nanocomposites, is analyzed.

In this work, the synthesis, selective chemical modifications, and self-assembly behavior in aqueous media of a novel poly(2-(dimethylamino)ethyl acrylate)20-b-poly(N-isopropylacrylamide)11-b-poly(oligo ethylene glycol methyl ether acrylate)18 (PDMAEA20-b-PNIPAM11-b-POEGA18) dual-responsive (pH and temperature) and triply hydrophilic amino-based triblock terpolymer are reported. The amine functional triblock terpolymer was synthesized by sequential reversible addition fragmentation chain transfer polymerization (RAFT) polymerization and molecularly characterized by size exclusion chromatography (SEC) and 1H-NMR spectroscopy that evidenced the success of the three-step polymerization scheme. The tertiary amine pendant groups of the PDMAEA block were chemically modified in order to produce the Q1PDMAEA20-b-PNIPAM11-b-POEGA18 as well as the Q6PDMAEA20-b-PNIPAM11-b-POEGA18 quaternized triblock terpolymers (Q1 and Q6 prefixes show the number of carbon atoms (C1 and C6) attached on the PDMAEA groups) using methyl iodide (CH3I) and 1-iodohexane (C6H13I) as the quaternizing agents and the SPDMAEA20-b-PNIPAM11-b-POEGA18 sulfobetainized triblock terpolymer using 1,3 propanesultone (C3H6O3S) as the sulfobetainization agent. The self-assembly properties of the triblock terpolymers in aqueous solutions upon varying temperature and solution pH were studied by light scattering and fluorescence spectroscopy experiments. The novel triblock terpolymers self-assemble into nanosized aggregates upon solution temperature rise above the nominal lower critical solution temperature (LCST) of the temperature-responsive PNIPAM block. The remarkable stimuli-responsive self-assembly behavior of the novel triblock terpolymers in aqueous media make them interesting candidates for biomedical applications in the fields of drug and gene delivery.

Stimuli-responsive polypeptides have gained attention because desirable bioactive properties can be easily imparted to them while keeping their biocompatibility and biodegradability intact. In this review, we summarize the most recent advances in various stimuli-responsive polypeptides (pH, reduction, oxidation, glucose, adenosine triphosphate (ATP), and enzyme) over the past five years. Various synthetic strategies exploited for advanced polypeptide-based materials are introduced, and their applicability in biomedical fields is discussed. The recent polypeptides imparted with new stimuli-responsiveness and their novel chemical and physical properties are explained in this review.

In this paper, recent developments in the chemical design of functional microgels are summarized. A wide range of available synthetic methods allows the incorporation of various reactive groups, charges, or biological markers inside the microgel network, thus controlling the deformation and swelling degree of the resulting smart microgels. These microgels can respond to various stimuli, such as temperature, pH, light, electric field, etc. and can show unique deformation behavior at the interface. Due to their switchability and interfacial properties, these smart microgels are being extensively explored for various applications, such as antifouling coatings, cell encapsulation, catalysis, controlled drug delivery, and tissue engineering.

Electrorheological (ER) and magnetorheological (MR) suspensions undergo a reverse phase transition from a liquid-like to solid-like state in response to an external electric or magnetic field, respectively. This paper briefly reviews various types of electro- or magneto-responsive materials from either polymeric or inorganic and hybrid composite materials. The fabrication strategies for ER/MR candidates and their ER/MR characteristics (particularly for ER fluids) are also included.

Although a number of tactics towards the fabrication and biomedical exploration of stimuli-responsive polymeric assemblies being responsive and adaptive to various factors have appeared, the controlled preparation of assemblies with well-defined physicochemical properties and tailor-made functions are still challenges. These responsive polymeric assemblies, which are triggered by stimuli, always exhibited reversible or irreversible changes in chemical structures and physical properties. However, simple drug/polymer nanocomplexes cannot deliver or release drugs into the diseased sites and cells on-demand due to the inevitable biological barriers. Hence, utilizing therapeutic or imaging agents-loaded stimuli-responsive block copolymer assemblies that are responsive to tumor internal microenvironments (pH, redox, enzyme, and temperature, etc.) or external stimuli (light and electromagnetic field, etc.) have emerged to be an important solution to improve therapeutic efficacy and imaging sensitivity through rationally designing as well as self-assembling approaches. In this review, we summarize a portion of recent progress in tumor and intracellular microenvironment responsive block copolymer assemblies and their applications in anticancer drug delivery and triggered release and enhanced imaging sensitivity. The outlook on future developments is also discussed. We hope that this review can stimulate more revolutionary ideas and novel concepts and meet the significant interest to diverse readers.

Star shaped segmented macromolecules constitute an interesting class of polymeric materials whose properties differ remarkably from those appearing in their linear counterparts. This review highlights the work done in the last decade, dealing with the self-assembly of star-shaped block copolymers and terpolymers of various topologies in aqueous media. This article focuses on a specific class of star shaped macromolecules designated as stimuli responsive. These stars bearblock/arms undergo sharp phase transitions upon responding to stimuli, such as temperature, pH, ionic strength and so forth. These transitions impose dramatic transformations on the morphology and, accordingly, in the functionality of the nanostructured associates. The number of arms, the specific functionality and topology of the different arm/blocks and the overall macromolecular architecture of the star polymer, significantly influence their behavior in terms of self-assembly and responsiveness.

Thermoresponsive polymers are a class of “smart” materials that have the ability to respond to a change in temperature; a property that makes them useful materials in a wide range of applications and consequently attracts much scientific interest. This review focuses mainly on the studies published over the last 10 years on the synthesis and use of thermoresponsive polymers for biomedical applications including drug delivery, tissue engineering and gene delivery. A summary of the main applications is given following the different studies on thermoresponsive polymers which are categorized based on their 3-dimensional structure; hydrogels, interpenetrating networks, micelles, crosslinked micelles, polymersomes, films and particles.

Heteroaggregation is the aggregation of mixed particle systems where the colloidal particles may differ in charge, size and chemical composition. The phenomenon of heteroaggregation is of great relevance in industrial processes and the natural environment. This review will focus on binary heteroaggregation where at least one of the particles is a stimulus-responsive smart particle. Aggregation under various conditions of pH, temperature, light and relative concentration can be induced by the careful manipulation of any one or more of these environmental conditions during the heteroaggregation of smart particles. Stimulus response provides the potential for reversibility from an aggregated to a stable system and exceptional control over inter-particle interactions. The significant fundamental and applied studies that have made an impact in this area will be discussed.

Helical structure is a sophisticated ubiquitous motif found in nature, in artificial polymers, and in supramolecular assemblies from microscopic to macroscopic points of view. Significant progress has been made in the synthesis and structural elucidation of helical polymers, nevertheless, a new direction for helical polymeric materials, is how to design smart systems with controllable helical chirality, and further use them to develop chiral functional materials and promote their applications in biology, biochemistry, medicine, and nanotechnology fields. This review summarizes the recent progress in the development of high-performance systems with tunable helical chirality on receiving external stimuli and discusses advances in their applications as drug delivery vesicles, sensors, molecular switches, and liquid crystals. Challenges and opportunities in this emerging area are also presented in the conclusion.

Poly[(organo)phosphazenes] are a unique class of extremely versatile polymers with a range of applications including tissue engineering and drug delivery, as hydrogels, shape memory polymers and as stimuli responsive materials. This review aims to divulge the basic principles of designing polyphosphazenes for drug and gene delivery and portray the huge potential of these extremely versatile materials for such applications. Polyphosphazenes offer a number of distinct advantages as carriers for bioconjugates; alongside their completely degradable backbone, to non-toxic degradation products, they possess an inherently and uniquely high functionality and, thanks to recent advances in their polymer chemistry, can be prepared with controlled molecular weights and narrow polydispersities, as well as self-assembled supra-molecular structures. Importantly, the rate of degradation/hydrolysis of the polymers can be carefully tuned to suit the desired application. In this review we detail the recent developments in the chemistry of polyphosphazenes, relevant to drug and gene delivery and describe recent investigations into their application in this field.