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Degradable Controlled-Release Polymers and Polymeric Nanoparticles: Mechanisms of Controlling Drug Release

1. Host−Guest Supramolecular Chemistry A 1.

Biomedical Applications of Supramolecular Systems Based on Host-Guest Interactions.

Supramolecular Amphiphiles Based on Host-Guest Molecular Recognition Motifs.

Importing self-repair or self-healing features into inert materials is of great relevance to material scientists, since it is expected to eliminate the necessity of replenishing a damaged material. Be it material chemistry or more specifically polymer chemistry, such materials have attracted the imagination of both material scientists and chemists. A stroll down the memory lane 70 years back, this might have sounded utopian. However with the current progress in supramolecular chemistry and the emergence of dynamic covalent and non-covalent chemistries, novel perspectives have been opened up to materials science towards the development of dynamic materials (DYNAMATS) and in particular dynamic polymers (DYNAMERS), with the ability to produce such species by custom made designs. Chemistry took giant strides to gain control over the structure and features of materials and, besides basic progress, to apply it for tailor-making matter for applications in our daily life. In that applied perspective, materials science plays a paramount role in shaping our present and in contributing to a sustainable future. The goal is to develop materials, which would be dynamic enough to carry out certain functions as effectively as in biological systems with, however, the freedom to recruit the powers of chemistry on a wider scale, without the limitation imposed by life. Material scientists and in particular polymer chemists may build on chemistry, physics and biology for bridging the gap to develop dynamic materials presenting a wide range of novel functionalities and to convert dreams into reality. In this current review we will focus on developments in the area of dynamic polymers, as a class of dynamic materials presenting self-healing features and, more generally, the ability to undergo adaptation under the effect of physical and/or chemical agents, and thus function as adaptive polymers or ADAPTAMERS.

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DYNAMERS: dynamic polymers as self-healing materials

3D printing alias additive manufacturing can transform 3D virtual models created by computer-aided design (CAD) into physical 3D objects in a layer-by-layer manner dispensing with conventional molding or machining. Since the incipiency, significant advancements have been achieved in understanding the process of 3D printing and the relationship of component, structure, property and application of the created objects. Because hydrogels are one of the most feasible classes of ink materials for 3D printing and this field has been rapidly advancing, this Review focuses on hydrogel designs and development of advanced hydrogel-based biomaterial inks and bioinks for 3D printing. It covers 3D printing techniques including laser printing (stereolithography, two-photon polymerization), extrusion printing (3D plotting, direct ink writing), inkjet printing, 3D bioprinting, 4D printing and 4D bioprinting. It provides a comprehensive overview and discussion of the tailorability of material, mechanical, physical, chemical and biological properties of hydrogels to enable advanced hydrogel designs for 3D printing. The range of hydrogel-forming polymers covered encompasses biopolymers, synthetic polymers, polymer blends, nanocomposites, functional polymers, and cell-laden systems. The representative biomedical applications selected demonstrate how hydrogel-based 3D printing is being exploited in tissue engineering, regenerative medicine, cancer research, in vitro disease modeling, high-throughput drug screening, surgical preparation, soft robotics and flexible wearable electronics. Incomparable by thermoplastics, thermosets, ceramics and metals, hydrogel-based 3D printing is playing a pivotal role in the design and creation of advanced functional (bio)systems in a customizable way. An outlook on future directions of hydrogel-based 3D printing is presented.

3D printing of hydrogels: Rational design strategies and emerging biomedical applications

Supramolecular materials held together by noncovalent interactions, such as hydrogen bonding, host-guest interactions, and electrostatic interactions, have great potential in material science. The unique reversibility and adaptivity of noncovalent intreractions have brought about fascinating new functions that are not available by their covalent counterparts and have greatly enriched the realm of functional materials. This review article aims to highlight the very recent and important progresses in the area of functional supramoleuclar materials, focusing on adaptive mechanical materials, smart sensors with enhanced selectivity, soft luminescent and electronic nanomaterials, and biomimetic and biomedical materials with tailored structures and functions. We cannot write a complete account of all the interesting work in this area in one article, but we hope that it can in a way reflect the current situation and future trends in this prosperously developing area of functional supramolecular materials.

25th anniversary article: reversible and adaptive functional supramolecular materials: "noncovalent interaction" matters.

In addition to conventional amphiphiles, an emerging research area is supra-amphiphiles, which are constructed on the basis of noncovalent interactions and dynamic covalent bonds. In this feature article, we have provided a general introduction to the concept, design principles, and topologies of supra-amphiphiles, starting from some rationally tailored building blocks. In addition, we highlight some progress in the functional assembly of supra-amphiphiles, such as responsive nanoscale carriers, antibacterial and antitumor agents, fluorescent-based chemical sensors, and enzyme mimics. The supra-amphiphile is a new bridge between colloidal science and supramolecular chemistry, and it is a field where we can make full use of our imaginative power.

Supra-amphiphiles: a new bridge between colloidal science and supramolecular chemistry.

Herein, we propose a new method for promoting covalent polymerization by supramolecular catalysts. To this end, we employed cucurbit[8]uril (CB[8]) as a supramolecular catalyst, and successfully prepared polyelectrolytes in an aqueous solution by taking advantage of the CB[8]-enhanced photodimerization of Brooker merocyanine moieties. Interestingly, 10 mol % CB[8] is enough to effectively catalyze this polymerization, because CB[8] can be spontaneously replaced by terminal groups from photodimerized products. In addition, the molecular weights of the obtained polyelectrolytes can be varied by the irradiation time or the monomer. By combining supramolecular catalysis and polymer chemistry, this line of research may enrich the methodology of polymerization and open up new horizons for supramolecular polymer chemistry.

Supramolecularly Catalyzed Polymerization: From Consecutive Dimerization to Polymerization.

The aromatic chromophores, for example, perylene diimides (PDIs) are well known for their desirable absorption and emission properties. However, their stacking nature hinders the exploitation of these properties and further applications. To fabricate emissive aggregates or solid-state materials, it has been common practice to decrease the degree of stacking of PDIs by incorporating substituents into the parent aromatic ring. However, such practice often involves difficultorganic synthesis with multiple steps. A supramolecular approach is established here to fabricate highly fluorescent and responsive soft materials, which has greatly decreases the number of required synthetic steps and also allows for a system with switchable photophysical properties. The highly fluorescent smart material exhibits great adaptivity and can be used as a supramolecular sensor for the rapid detection of spermine with high sensitivity and selectivity, which is crucial for the early diagnosis of malignant tumors.

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Yuetong Kang

Papers

25th anniversary article: reversible and adaptive functional supramolecular materials: "noncovalent interaction" matters.

Supra-amphiphiles: a new bridge between colloidal science and supramolecular chemistry.

Supramolecularly Catalyzed Polymerization: From Consecutive Dimerization to Polymerization.

A supramolecular approach to fabricate highly emissive smart materials

Enzyme-responsive polymer assemblies constructed through covalent synthesis and supramolecular strategy