Fabrication of short peptide cages by interfacial self-assembly on CaCO3 templates

Lu, Feng; Ren, Peng; Hao, Linna; Dong, Qianqian; Li, Jieling; Jian, Honglei; Wang, Meiyue; Li, Xin; Wang, Anhe

doi:10.1016/j.colsurfa.2019.04.048

Cited by 13 publications

(8 citation statements)

References 45 publications

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“…Our current study provides a thorough understanding of the catalytic mechanism of thermolysin, in particular, a new methodology for bottom-up nanofabrication of future soft-gel materials, and has instructive significance on the regulation of peptide sequences, secondary structure, morphology, and mechanical property of self-assembled hydrogels with precise design and control in molecular level by thermolysin and functional applications of peptide materials. [49][50][51][52][53][54]…”

Section: Resultsmentioning

confidence: 99%

Role of Thermolysin in Catalytic-Controlled Self-Assembly of Fmoc-Dipeptides

et al. 2020

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In recent years, short peptide self-assembled materials, prepared under the control of the thermolysin catalyst, have been investigated extensively and shown to acquire various morphologies and functions as building blocks for a wide range of biomaterials and device applications. However, the role played by thermolysin in this enzymatically triggered peptide self-assembly is still ambiguous. Herein, we designed a series of Fmoc-dipeptide amphiphiles to explore the catalytic role of thermolysin. The results from our experiments and computational simulations showed that hydrophobicity and amino acid sequences of substrates have a significant correlation with thermolysin actions, including the binding capacity and catalytic efficiency. Specifically, thermolysin favors a specific substrate pattern with a hydrophilic amino acid in the first residue and hydrophobic amino acid in the second residue. Moreover, thermolysin catalyzed reactions are bidirectional and could move toward hydrolysis or condensation based on the design of its diverse substrates (peptides). However, the specificity of the enzyme action lies in the major site of its cleavage, which is the terminal hydrophobic or bulky amino side chains. We designed a two-step reaction, taking advantage of the bidirectional catalytic actions of thermolysin, to modify the sequence of N α-fluorenylmethoxycarbonyl (Fmoc)-dipeptide from Fmoc-YL-COOH to Fmoc-YY-NH 2 and treated with thermolysin, which resulted in the enzyme-catalyzed gel-sol-gel transition. This work has an instructive significance in the regulation of peptide sequences, secondary amino acid structures, morphology, and the mechanical property of self-assembled hydrogels with precise design and control at the molecular level via thermolysin catalysis.

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Section: Resultsmentioning

confidence: 99%

Role of Thermolysin in Catalytic-Controlled Self-Assembly of Fmoc-Dipeptides

et al. 2020

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“…In a related study, Bai et al devised an interesting application of ENS for making peptide cages. 376 Specifically, the authors absorbed thermolysin on porous CaCO 3 microparticles to catalyze the condensation reaction of Fmoc-Y (2) and L-NH 2 in a water/hexane emulsion. This biphasic system limits the self-assembly of Fmoc-YL-NH 2 on CaCO 3 surface.…”

Section: Proteasesmentioning

confidence: 99%

“…This model system would be extremely useful if it can mimic the ENS processes that occur on a cell surface. In a related study, Bai et al devised an interesting application of ENS for making peptide cages . Specifically, the authors absorbed thermolysin on porous CaCO 3 microparticles to catalyze the condensation reaction of Fmoc-Y ( 2 ) and L-NH 2 in a water/hexane emulsion.…”

Section: Enzymatic Noncovalent Synthesis In Cell-free Conditionsmentioning

confidence: 99%

Enzymatic Noncovalent Synthesis

et al. 2020

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Enzymatic reactions and noncovalent (i.e., supramolecular) interactions are two fundamental nongenetic attributes of life. Enzymatic noncovalent synthesis (ENS) refers to a process where enzymatic reactions control intermolecular noncovalent interactions for spatial organization of higher-order molecular assemblies that exhibit emergent properties and functions. Like enzymatic covalent synthesis (ECS), in which an enzyme catalyzes the formation of covalent bonds to generate individual molecules, ENS is a unifying theme for understanding the functions, morphologies, and locations of molecular ensembles in cellular environments. This review intends to provide a summary of the works of ENS within the last decade and emphasize ENS for functions. After comparing ECS and ENS, we describe a few representative examples where nature uses ENS, as a rule of life, to create the ensembles of biomacromolecules for emergent properties/functions in a myriad of cellular processes. Then, we focus on ENS of man-made (synthetic) molecules in cell-free conditions, classified by the types of enzymes. After that, we introduce the exploration of ENS of man-made molecules in the context of cells by discussing intercellular, peri/intracellular, and subcellular ENS for cell morphogenesis, molecular imaging, cancer therapy, and other applications. Finally, we provide a perspective on the promises of ENS for developing molecular assemblies/processes for functions. This review aims to be an updated introduction for researchers who are interested in exploring noncovalent synthesis for developing molecular science and technologies to address societal needs.

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“…programmed self-assembly became a key facilitator in the fabrication of innovative compartmentalized nanostructures, making use of non-covalent interactions among distinct molecular building blocks, 15,16 and/or exploiting specic templates or stimuli to modulate their self-assembly process. [17][18][19] For example, discrete self-assembled molecular cages have also been reported, in which the restrained compartments were exploited for selective chemical reactions and processes, as well as responsive containers. [20][21][22][23][24][25][26] More recently, conned space has also been obtained via self-assembly of nanoparticles (NPs).…”

Section: Valentinamentioning

confidence: 99%