Supramolecular gels are formed by the self-assembly of small molecules under the influence of various non-covalent interactions. As the interactions are individually weak and reversible, it is possible to perturb the gels easily, which in turn enables fine tuning of their properties. Synthetic supramolecular gels are kinetically trapped and usually do not show time variable changes in material properties after formation. However, such materials potentially become switchable when exposed to external stimuli like temperature, pH, light, enzyme, redox, and chemical analytes resulting in reconfiguration of gel matrix into a different type of network. Such transformations allow gel-to-gel transitions while the changes in the molecular aggregation result in alteration of physical and chemical properties of the gel with time. Here, we discuss various methods that have been used to achieve gel-to-gel transitions by modifying a pre-formed gel material through external perturbation. We also describe methods that allow time-dependent autonomous switching of gels into different networks enabling synthesis of next generation functional materials. Dynamic modification of gels allows construction of an array of supramolecular gels with various properties from a single material which eventually extend the limit of applications of the gels. In some cases, gel-to-gel transitions lead to materials that cannot be accessed directly. Finally, we point out the necessity and possibility of further exploration of the field.

/pdf/stimuli-responsive-dynamic-transformations-in-supramolecular-1kaeb90tu7.pdf

Stimuli responsive dynamic transformations in supramolecular gels

The spread of antibiotic resistance to humans and potential protection strategies.

This review provides a summary of recent progress in the development of different nano-platforms for the efficient synergistic effect between photodynamic therapy and chemotherapy. In particular, this review focuses on various methods in which photosensitizers and chemotherapeutic agents are co-delivered to the targeted tumor site. In many cases, the photosensitizers act as drug carriers, but this review, also covers different types of appropriate nanocarriers that aid in the delivery of photosensitizers to the tumor site. These nanocarriers include transition metal, silica and graphene-based materials, liposomes, dendrimers, polymers, metal–organic frameworks, nano emulsions, and biologically derived nanocarriers. Many studies have demonstrated various benefits from using these nanocarriers including enhanced water solubility, stability, longer circulation times, and higher accumulation of therapeutic agents/photosensitizers at tumor sites. This review also describes novel approaches from different research groups that utilize various targeting strategies to increase treatment efficacy through simultaneous photodynamic therapy and chemotherapy.

https://www.mdpi.com/1999-4923/14/2/322/pdf?version=1644571180

Synergic Antitumor Effect of Photodynamic Therapy and Chemotherapy Mediated by Nano Drug Delivery Systems

Hofmeister effects play a crucial role in nanoscience by affecting the physicochemical and biochemical processes. Thus far, numerous wonderful applications from various aspects of nanoscience have been developed based on the mechanism of Hofmeister effects, such as hydrogel/aerogel engineering, battery design, nanosynthesis, nanomotors, ion sensors, supramolecular chemistry, colloid and interface science, nanomedicine, and transport behaviors, etc. In this review, for the first time, the progress of applying Hofmeister effects is systematically introduced and summarized in nanoscience. It is aimed to provide a comprehensive guideline for future researchers to design more useful Hofmeister effects-based nanosystems.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202302057

Hofmeister Effects Shine in Nanoscience.

Thermoresponsive supramolecular assemblies have been extensively explored in diverse formats, from injectable hydrogels to nanoscale carriers, for a variety of applications including drug delivery, tissue engineering and thermo-controlled catalysis. Understanding the molecular bases behind thermal sensitivity of materials is fundamentally important for the rational design of assemblies with optimal combination of properties and predictable tunability for specific applications. In this review, we summarize the recent advances in this area with a specific focus on the parameters and factors that influence thermoresponsive properties of soft materials. We summarize and analyze the effects of structures and architectures of molecules, hydrophilic and lipophilic balance, concentration, components and external additives upon the thermoresponsiveness of the corresponding molecular assemblies.

Molecular bases for temperature sensitivity in supramolecular assemblies and their applications as thermoresponsive soft materials.

A primary component of all known bacterial cell walls is the peptidoglycan (PG) layer, which is composed of repeating units of sugars connected to short and unusual peptides. The various steps within PG biosynthesis are targets of potent antibiotics as proper assembly of the PG is essential for cellular growth and survival. Synthetic mimics of PG have proven to be indispensable tools to study the bacterial cell structure, growth, and remodeling. Yet, a common component of PG, meso-diaminopimelic acid (m-DAP) at the third position of the stem peptide, remains challenging to access synthetically and is not commercially available. Here, we describe the synthesis and metabolic processing of a selenium-based bioisostere of m-DAP (selenolanthionine) and show that it is installed within the PG of live bacteria by the native cell wall crosslinking machinery in mycobacterial species. This PG probe has an orthogonal release mechanism that could be important for downstream proteomics studies. Finally, we describe a bead-based assay that is compatible with high-throughput screening of cell wall enzymes. We envision that this probe will supplement the current methods available for investigating PG crosslinking in m-DAP-containing organisms. 

Metabolic Processing of Selenium-Based Bioisosteres of meso-Diaminopimelic Acid in Live Bacteria

Enzyme-Triggered Nanomaterials and Their Applications

The propensity of broad-spectrum antibiotics to indiscriminately kill both pathogenic and beneficial bacteria has a profound impact on the spread of resistance across multiple bacterial species. Alternative approaches that narrow antibacterial specificity towards desired pathogenic bacterial population are of great interest. Here, we report an enzyme-responsive antibiotic-loaded nanoassembly strategy for narrow delivery of otherwise broad-spectrum antibiotics. We specifically target Staphylococcus aureus (S. aureus), an important blood pathogen that secretes PC1 β-lactamases. Our nanoassemblies selectively eradicate S. aureus grown in vitro with other bacteria, highlighting its potential capability in targeting the desired pathogenic bacterial population.

https://pubs.rsc.org/en/content/articlepdf/2020/nr/d0nr04886k

Supramolecular antibiotics: a strategy for conversion of broad-spectrum to narrow-spectrum antibiotics for Staphylococcus aureus

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Molecular bases for temperature sensitivity in supramolecular assemblies and their applications as thermoresponsive soft materials.

Metabolic Processing of Selenium-Based Bioisosteres of meso-Diaminopimelic Acid in Live Bacteria

Enzyme-Triggered Nanomaterials and Their Applications

Supramolecular antibiotics: a strategy for conversion of broad-spectrum to narrow-spectrum antibiotics for Staphylococcus aureus