Preparation of Amylose-Carboxymethyl Cellulose Conjugated Supramolecular Networks by Phosphorylase-Catalyzed Enzymatic Polymerization

Kadokawa, Jun‐ichi; Shoji, Takuya; Yamamoto, Katsuhiro

doi:10.3390/catal9030211

Cited by 6 publications

(3 citation statements)

References 35 publications

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“…Lower ratios of PCL give rise to the hierarchical nanoarchitecture of larger networks, mostly composed of amylosic double helixes, leading to the formation of supramolecular hydrogels from the reaction mixtures. In contrast, the presence of higher ratios of PCL induces Another approach to construct amylosic supramolecular networks through the vinetwining polymerization process has been investigated through the GP-catalyzed enzymatic polymerization in the presence of PCL using Glc 7 primer-modified Pg-GA and NaCMC (Figure 9) [50][51][52]. PCL/primer feed ratios strongly affect the macroscopic structures of the resulting amylosic supramolecular networks as shown in Figure 10.…”

Section: Hierarchical Nanoarchitecture Of Amylosic Supramolecular Net...mentioning

confidence: 99%

“…In contrast, the presence of higher ratios of PCL induces smaller nanonetworks to form, largely comprising the amylosic inclusion complexes with PCL, according to the vine-twining polymerization process, giving rise to aggregates in the reaction mixtures. Another approach to construct amylosic supramolecular networks through the vinetwining polymerization process has been investigated through the GP-catalyzed enzymatic polymerization in the presence of PCL using Glc7 primer-modified Pg-GA and NaCMC (Figure 9) [50][51][52]. PCL/primer feed ratios strongly affect the macroscopic structures of the resulting amylosic supramolecular networks as shown in Figure 10.…”

Section: Hierarchical Nanoarchitecture Of Amylosic Supramolecular Net...mentioning

confidence: 99%

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Fabrication of Nanostructured Supramolecules through Helical Inclusion of Amylose toward Hydrophobic Polyester Guests, Biomimetically through Vine-Twining Polymerization Process

Kadokawa

2023

Biomimetics

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This review article presents the biomimetic helical inclusion of amylose toward hydrophobic polyesters as guests through a vine-twining polymerization process, which has been performed in the glucan phosphorylase (GP)-catalyzed enzymatic polymerization field to fabricate supramolecules and other nanostructured materials. Amylose, which is a representative abundant glucose polymer (polysaccharide) with left-handed helical conformation, is well known to include a number of hydrophobic guest molecules with suitable geometry and size in its cavity to construct helical inclusion complexes. Pure amylose is prepared through enzymatic polymerization of α-d-glucose 1-phosphate as a monomer using a maltooligosaccharide as a primer, catalyzed by GP. It is reported that the elongated amylosic chain at the nonreducing end in enzymatic polymerization twines around guest polymers with suitable structures and moderate hydrophobicity, which is dispersed in aqueous polymerization media, to form amylosic nanostructured inclusion complexes. As the image of this system is similar to how vines of a plant grow around a support rod, this polymerization has been named ‘vine-twining polymerization’. In particular, the helical inclusion behavior of the enzymatically produced amylose toward hydrophobic polyesters depending on their structures, e.g., chain lengths and substituents, has been systematically investigated in the vine-twining polymerization field. Furthermore, amylosic supramolecular network materials, such as hydrogels, are fabricated through vine-twining polymerization by using copolymers, where hydrophobic polyester guests or maltooligosaccharide primers are covalently modified on hydrophilic main-chain polymers. The vine-twining polymerization using such copolymers in the appropriate systems induces the formation of amylosic nanostructured inclusion complexes among them, which act as cross-linking points, giving rise to supramolecular networks at the nanoscale. The resulting materials form supramolecular hydrogels, films, and microparticles.

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Section: Hierarchical Nanoarchitecture Of Amylosic Supramolecular Net...mentioning

confidence: 99%

Section: Hierarchical Nanoarchitecture Of Amylosic Supramolecular Net...mentioning

confidence: 99%

Fabrication of Nanostructured Supramolecules through Helical Inclusion of Amylose toward Hydrophobic Polyester Guests, Biomimetically through Vine-Twining Polymerization Process

Kadokawa

2023

Biomimetics

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“…These results were in accordance with the previous study [22], in which the chain of glycogen was elongated by phosphorylase and then the elongated chains self-assembled and formed the double helix through hydrogen bonds. Moreover, enzymatic glucan grafting was successfully performed on chitosan [23,24], cellulose [25] and carboxymethyl cellulose [26].…”

Section: Xrd Analysismentioning

confidence: 99%

Fabrication, Structure and Functional Characterizations of pH-Responsive Hydrogels Derived from Phytoglycogen

Liu

Chen

et al. 2021

Foods

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The pH-responsive hydrogels were obtained through successive carboxymethylation and phosphorylase elongatation of phytoglycogen and their structure and functional characterizations were investigated. Phytoglycogen (PG) was first carboxymethylated to obtain carboxymethyl phytoglycogen (CM-PG) with degree of substitution (DS) at 0.15, 0.25, 0.30, and 0.40, respectively. Iodine staining and X-ray diffraction analysis suggested that the linear glucan chains were successfully phosphorylase-elongated from the non-reducing ends at the CM-PG surface and assembled into the double helical segments, leading to formation of the hydrogel. The DS of CM-PG significantly influenced elongation of glucan chains. Specifically, fewer glucan chains were elongated for CM-PG with higher DS and the final glucan chains were shorter, resulting in lower gelation rate of chain-elongated CM-PG and lower firmness of the corresponding hydrogels. Scanning electron microscope observed that the hydrogels exhibited a porous and interconnected morphology. The swelling ratio and volume of hydrogels was low at pH 3–5 and then became larger at pH 6–8 due to electrostatic repulsion resulting from deprotonated carboxymethyl groups. Particularly, the hydrogel prepared from chain-elongated CM-PG (DS = 0.25) showed the highest sensitivity to pH. These results suggested that phosphorylase-treated CM-PG formed the pH-responsive hydrogel and that the elongation degree and the properties of hydrogels depended on the carboxymethylation degree. Thus, it was inferred that these hydrogels was a potential carrier system of bioactive substances for their targeted releasing in small intestine.

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Hydrophobization of surfaces on cellulose nanofibers by enzymatic grafting of partially 2-deoxygenated amylose

Totani,

Anai,

Kadokawa

2024

Carbohydrate Polymers

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Preparation of Amylose-Carboxymethyl Cellulose Conjugated Supramolecular Networks by Phosphorylase-Catalyzed Enzymatic Polymerization

Cited by 6 publications

References 35 publications

Fabrication of Nanostructured Supramolecules through Helical Inclusion of Amylose toward Hydrophobic Polyester Guests, Biomimetically through Vine-Twining Polymerization Process

Fabrication of Nanostructured Supramolecules through Helical Inclusion of Amylose toward Hydrophobic Polyester Guests, Biomimetically through Vine-Twining Polymerization Process

Fabrication, Structure and Functional Characterizations of pH-Responsive Hydrogels Derived from Phytoglycogen

Hydrophobization of surfaces on cellulose nanofibers by enzymatic grafting of partially 2-deoxygenated amylose

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