Supramolecular Shear-Thinning Glycopeptide Hydrogels for Injectable Enzyme Prodrug Therapy Applications

Sakamoto, Yusuke; Suehiro, Fumi; Akiba, Isamu; Nishimura, Tomoki

doi:10.1021/acs.langmuir.2c00504

Cited by 5 publications

(5 citation statements)

References 62 publications

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“…These enzyme-loaded hydrogels can transform the prodrugs into anticancer drugs and can be employed as injectable biocatalytic reactors [Figure 25, (62)]. 144 LMWGs based on tris-urea with hydrophilic glucosides arranged onto the circle of the hydrophobic part were introduced. The formed hydrogel demonstrated the gel-to-sol transition in response to lectin and anion.…”

Section: Glycolipid Gelators Based On Monosaccharidesmentioning

confidence: 99%

“…This supramolecular hydrogel with biocatalytic activity can be used for enzyme prodrug therapy. These enzyme-loaded hydrogels can transform the prodrugs into anticancer drugs and can be employed as injectable biocatalytic reactors [Figure , ( 62 )] …”

Section: Glycolipid-based Gelatorsmentioning

confidence: 99%

“…These enzyme-loaded hydrogels can transform the prodrugs into anticancer drugs and can be employed as injectable biocatalytic reactors [ Figure 25 , ( 62 )]. 144 …”

Section: Glycolipid-based Gelatorsmentioning

confidence: 99%

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Harnessing Glycolipids for Supramolecular Gelation: A Contemporary Review

Holey,

Nayak

2024

ACS Omega

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Within the scope of this review, our exploration spans diverse facets of amphiphilic glycolipid-based low-molecular-weight gelators (LMWGs). This journey explores glycolipid synthesis, selfassembly, and gelation with tailorable properties. It begins by examining the design of glycolipids and their influence on gel formation. Following this, a brief exploration of several gel characterization techniques adds another layer to the understanding of these materials. The final section is dedicated to unraveling the various applications of these glycolipid-based supramolecular gels. A meticulous analysis of available glycolipid gelators and their correlations with desired properties for distinct applications is a pivotal aspect of their investigation. As of the present moment, there exists a notable absence of a review dedicated exclusively to glycolipid gelators. This study aims to bridge this critical gap by presenting an overview that provides novel insights into their unique properties and versatile applications. This holistic examination seeks to contribute to a deeper understanding of molecular design, structural characteristics, and functional applications of glycolipid gelators by offering insights that can propel advancements in these converging scientific disciplines. Overall, this review highlights the diverse classifications of glycolipid-derived gelators and particularly emphasizes their capacity to form gels.

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Section: Glycolipid Gelators Based On Monosaccharidesmentioning

confidence: 99%

Section: Glycolipid-based Gelatorsmentioning

confidence: 99%

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Harnessing Glycolipids for Supramolecular Gelation: A Contemporary Review

Holey,

Nayak

2024

ACS Omega

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“…These gels are susceptible to being disrupted by applied mechanical forces, which can change in the mechanical strength of the hydrogel or induce a transition from the gel to sol state. [151][152][153][154][155][156] A supramolecular hydrogel composed of 𝜋-𝜋 and hydrogen bonding interactions was prepared and it was observed that the hydrogel could break its molecular assembled state under external mechanical force and transition from a gel to sol state. Although its mechanical strength was relatively weak, it exhibited good strain recovery.…”

Section: Supramolecular Hydrogels Triggered By Mechanicsmentioning

confidence: 99%

Bioinspired Supramolecular Hydrogel from Design to Applications

Gao,

Yang,

Song

2023

Small Methods

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Nature offers a wealth of opportunities to solve scientific and technological issues based on its unique structures and function. The dynamic non‐covalent interaction is considered to be the main base of living functions of creatures including humans, animals, and plants. Supramolecular hydrogels formed by non‐covalent bonding interactions has become a unique platform for constructing promising materials for medicine, energy, electronic, and biological substitute. In this review, the self‐assemble principle of supramolecular hydrogels is summarized. Next, the stimulation of external environment that triggers the assembly or disassembly of supramolecular hydrogels are recapitulated, including temperature, mechanics, light, pH, ions, etc. The main applications of bioinspired supramolecular hydrogels in terms of bionic objects including humans, animals, and plants are also described. Although so many efforts are done for revealing the synergized mechanism of the function and non‐covalent interactions on the supramolecular hydrogel, the complexity and variability between stimulus and non‐covalent bonding in the supramolecular system still require impeccable theories. As an outlook, the bioinspired supramolecular hydrogel is just beginning to exhibit its great potential in human life, offering significant opportunities in drug delivery and screening, implantable devices and substitutions, tissue engineering, micro‐fluidic devices, and biosensors.

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“…To date, various artificial bioreactors have been developed and utilized to understand a wide range of catalytic transformations under confinement. These include liposomes, , microemulsions, , polymersomes, , polymeric capsules, , metal–organic frameworks (MOFs), , covalent organic frameworks (COFs), , hydrogels, , and deoxyribonucleic acid (DNA) nanostructures. , These robust architectures not only stabilize the native conformations of enzymes and protect them from harmful external conditions such as acidic pH, temperature, protease digestion, and denaturation, but also enhance the enzymatic activity via stabilization of the active site, modulation of chemical activity, and enhanced mass transport. For example, Liang et al demonstrated enhanced activity of encapsulated catalase and urease inside the porous cavity of hydrophilic MOF, while negligible or no activity was observed inside hydrophobic MOF .…”

Section: Introductionmentioning

confidence: 99%

Synthetic Protocell as Efficient Bioreactor: Enzymatic Superactivity and Ultrasensitive Glucose Sensing in Urine

Saini

Mukherjee

2022

ACS Appl. Mater. Interfaces

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It is believed that membraneless cellular condensates play a critical role in accelerating various slow and thermodynamically unfavorable biochemical processes. However, the exact mechanisms behind the enhanced activity within biocondensates remain poorly understood. Here, we report the fabrication of a high-performance integrated cascade bioplatform based on synthetic droplets for ultrasensitive glucose sensing. Using a horseradish peroxidase (HRP) and glucose oxidase (GOx) cascade pair, we report an unprecedented enhancement in the catalytic activity of HRP inside the synthetic membraneless droplet. Liquidlike membraneless droplets have been prepared via multivalent electrostatic interactions between adenosine triphosphate (ATP) and poly(diallyldimethylammonium chloride) (PDAD-MAC) in an aqueous medium. Compartmentalized enzymes (GOx/HRP@Droplet) exhibit high encapsulation efficiency, low leakage, prolong retention of activity, and exceptional stability toward protease digestion. Using an HRP@Droplet composite, we have shown that the enzymatic reaction within the droplet follows the classical Michaelis−Menten model. Our findings reveal remarkable enhancement in the catalytic activity of up to 100-and 51fold for HRP@Droplet and GOx/HRP@Droplet, respectively. These enhanced activities have been explained on the basis of increased local concentrations of enzymes and substrates, along with altered conformations of sequestered enzymes. Furthermore, we have utilized highly efficient and recyclable GOx/HRP@Droplet composite to demonstrate ultrasensitive glucose sensing with a limit of detection of 228 nM. Finally, the composite platform has been exploited to detect glucose in spiked urine samples in solution and filter paper. Our present study illustrates the unprecedented activity of the compartmentalized enzymes and paves the way for next-generation composite bioreactors for a wide range of applications.

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Supramolecular Shear-Thinning Glycopeptide Hydrogels for Injectable Enzyme Prodrug Therapy Applications

Cited by 5 publications

References 62 publications

Harnessing Glycolipids for Supramolecular Gelation: A Contemporary Review

Harnessing Glycolipids for Supramolecular Gelation: A Contemporary Review

Bioinspired Supramolecular Hydrogel from Design to Applications

Synthetic Protocell as Efficient Bioreactor: Enzymatic Superactivity and Ultrasensitive Glucose Sensing in Urine

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