Effects of hydrogen bonds on the single-chain mechanics of chitin

Lu, Qian; Guo, Xin; Zhang, Kai; Yu, Miao

doi:10.1039/d2cp02907c

Cited by 7 publications

(6 citation statements)

References 62 publications

(111 reference statements)

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“…The quantum mechanical modified freely jointed chain (QM-FJC) model has been successfully used to describe the theoretical backbone elasticity of a single cellulose/amylose chain. , As shown in Figure B, the experimental F-E curves may be superimposed with the QM-FJC model at l k = 0.514 nm (see the Supporting Information and Figure S2 for details), demonstrating that the single-chain backbone elasticity of chitosans in DMSO was obtained. Due to the ability of DMSO to disrupt intra-chain H-bonds of these chitosans, these four polysaccharides show the same single-chain backbone elasticity in DMSO.…”

Section: Results and Discussionmentioning

confidence: 98%

Effects of the Degree of Deacetylation on the Single-Molecule Mechanics of Chitosans

Zhang

Guo

et al. 2023

J. Phys. Chem. B

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Chitosan is one of the most prevalent biomass materials, and its physicochemical and biological characteristics, such as solubility, crystallinity, flocculation ability, biodegradability, and amino-related chemical processes, are directly connected to the degree of deacetylation (DD). However, the specifics about the effects of the DD on the characteristics of chitosan are still unclear up to now. In this work, atomic force microscopy-based single-molecule force spectroscopy was used to study the role of the DD in the single-molecule mechanics of chitosan. Even though the DD varies largely (17% ≤ DD ≤ 95%), the experimental results demonstrate that the chitosans exhibit the same natural (in nonane) and backbone (in dimethyl sulfoxide (DMSO)) single-chain elasticity. This suggests that chitosans have the same intra-chain hydrogen bond (H-bond) state in nonane and to which these H-bonds can be eliminated in DMSO. However, when the experiments are carried out in ethylene glycol (EG) and water, the single-chain mechanics are increased with the increases of the DD. The energy consumed to stretch chitosans in water is larger than that in EG, indicating that amino can form a strong interaction with water and induce the formation of the binding water around the sugar rings. The strong interaction between water and amino may be the key factor for the well solubility and chemical activity of chitosan. The results of this work are anticipated to provide fresh light on the significant role played by the DD and water in the structures and functions of chitosan at the single molecular level.

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Section: Results and Discussionmentioning

confidence: 98%

Effects of the Degree of Deacetylation on the Single-Molecule Mechanics of Chitosans

Zhang

Guo

et al. 2023

J. Phys. Chem. B

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“…Concurrently, the polymers situated on the substrate underwent controlled stretching at a rate of 2 µm/s. These experiments took place in a temperature-controlled room, maintaining a constant temperature of 24 • C [35][36][37][38].…”

Section: Methodsmentioning

confidence: 99%

Exploring Novel Sensor Design Ideas through Concentration-Induced Conformational Changes in PEG Single Chains

Yu,

Jiang,

Lai

et al. 2024

Sensors

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Polyethylene glycol (PEG) is an artificial polymer with good biocompatibility and a low cost, which has a wide range of applications. In this study, the dynamic response of PEG single chains to different ion concentrations was investigated from a microscopic point of view based on single-molecule force spectroscopy, revealing unique interactions that go beyond the traditional sensor-design paradigm. Under low concentrations of potassium chloride, PEG single chains exhibit a gradual reduction in rigidity, while, conversely, high concentrations induce a progressive increase in rigidity. This dichotomy serves as the cornerstone for a profound understanding of PEG conformational dynamics under diverse ion environments. Capitalizing on the remarkable sensitivity of PEG single chains to ion concentration shifts, we introduce innovative sensor-design ideas. Rooted in the adaptive nature of PEG single chains, these sensor designs extend beyond the traditional applications, promising advancements in environmental monitoring, healthcare, and materials science.

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“…Besides, a similar case, in which the shift in the nanofiber groups was larger than that of the nanoparticle groups, was also obtained in MeOD-d 4 / D 2 O, but the shift space in this condition was smaller than that in DMSO/D 2 O (e.g., ∼12 cm −1 in MeOD-d 4 /D 2 O vs ∼50 cm −1 in DMSO/D 2 O for Fmoc-Tyr-OH), indicating that the solvents may have some effects on hydrogen bonds, probably attributed to the hydrogen bond breaking nature of DMSO. 57,58 Moreover, the existence of a hydrogen bond network can also explain the much higher CACs of Fmoc-Tyr-OH than those of other groups (Figures S5f and S6f). DMSO or MeOH could competitively form hydrogen bonds with blocks, which impacted the generation of intermolecular hydrogen bonds between Fmoc-Tyr-OH, hindering their selfassembly.…”

Section: ■ Introductionmentioning

confidence: 91%

Structural Transformation of Coassembled Fmoc-Protected Aromatic Amino Acids to Nanoparticles

Wang,

Ménard-Moyon,

Bianco

2024

ACS Appl. Mater. Interfaces

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Materials made of assembled biomolecules such as amino acids have drawn much attention during the past decades. Nevertheless, research on the relationship between the chemical structure of building block molecules, supramolecular interactions, and self-assembled structures is still necessary. Herein, the selfassembly and the coassembly of fluorenylmethoxycarbonyl (Fmoc)-protected aromatic amino acids (tyrosine, tryptophan, and phenylalanine) were studied. The individual self-assembly of Fmoc-Tyr-OH and Fmoc-Phe-OH in water formed nanofibers, while Fmoc-Trp-OH self-assembled into nanoparticles. Moreover, when Fmoc-Tyr-OH or Fmoc-Phe-OH was coassembled with Fmoc-Trp-OH, the nanofibers were transformed into nanoparticles. UV−vis spectroscopy, Fourier transform infrared spectroscopy, and fluorescence spectroscopy were used to investigate the supramolecular interactions leading to the self-assembled architectures. π−π stacking and hydrogen bonding were the main driving forces leading to the self-assembly of Fmoc-Tyr-OH and Fmoc-Phe-OH forming nanofibers. Further, a mechanism involving a two-step coassembly process is proposed based on nucleation and elongation/growth to explain the structural transformation. Fmoc-Trp-OH acted as a fiber inhibitor to alter the molecular interactions in the Fmoc-Tyr-OH or Fmoc-Phe-OH self-assembled structures during the coassembly process, locking the coassembly in the nucleation step and preventing the formation of nanofibers. This structural transformation is useful for extending the application of amino acid self-or coassembled materials in different fields. For example, the amino acids forming nanofibers could be applied for tissue engineering, while they could be exploited as drug nanocarriers when they form nanoparticles.

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Effects of hydrogen bonds on the single-chain mechanics of chitin

Abstract: Water is essential in the evolution of life and plays an important role in the structure and function of the basic substances of life, such as proteins and DNA. However,...

Cited by 7 publications

References 62 publications

Effects of the Degree of Deacetylation on the Single-Molecule Mechanics of Chitosans

Effects of the Degree of Deacetylation on the Single-Molecule Mechanics of Chitosans

Exploring Novel Sensor Design Ideas through Concentration-Induced Conformational Changes in PEG Single Chains

Structural Transformation of Coassembled Fmoc-Protected Aromatic Amino Acids to Nanoparticles

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