Moldable Material from ε-Poly-<scp>l</scp>-lysine and Lignosulfonate: Mechanical and Self-Healing Properties of a Bio-Based Polyelectrolyte Complex

Ushimaru, Kazunori; Hamano, Yoshimitsu; Morita, Tomotake; Fukuoka, Tokuma

doi:10.1021/acsomega.9b00968

Cited by 12 publications

(4 citation statements)

References 35 publications

(93 reference statements)

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“…Syntheses of polymers from the AMDP raw material were investigated. ε-PL, which has primary amino groups, is a polypeptide obtained by microbial fermentation and is biodegradable; it is usually combined with other polymers to form films. − Herein, we attempted to prepare ε-PL-based films via condensation reactions with different AMDP ratios (0.2, 2.4, and 7.2 wt % relative to the ε-PL weight) (Figure a). The viscous ε-PL liquid reacted with AMDP in the presence of the condensing agent DMT-MM, and the product was purified by dialysis and lyophilized to produce powdered samples.…”

Section: Resultsmentioning

confidence: 99%

Melanin Upcycling: Creation of Polymeric Materials from Melanin Decomposition Products

Morita,

Matsuura,

Izawa

et al. 2024

ACS Sustainable Chem. Eng.

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Melanin is a widely occurring biopolymer and has been the subject of much research, especially in dermatology. However, from a resource perspective, melanin is still an unutilized biomass because of its complex three-dimensional cross-linked structure, which makes it challenging to handle. Here, we demonstrate melanin upcycling by decomposing melanin and preparing polymeric materials from its products. A detailed study of the chemical decomposition products of artificial melanin, i.e., polydopamine, reveals that the melanin decomposition products are mainly oligomeric pyrrole derivatives containing carboxylic acids. Furthermore, decomposition experiments using natural melanin extracted from cuttlefish ink revealed that the composition of melanin decomposition products is almost identical regardless of the melanin source. We proposed a melanin decomposition mechanism and demonstrated the preparation of biobased polymer films and particles from melanin decomposition products. The use of melanin decomposition products as building blocks for material preparation is expected to lead to the development of new biodegradable polymers from biomass.

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Section: Resultsmentioning

confidence: 99%

Melanin Upcycling: Creation of Polymeric Materials from Melanin Decomposition Products

Morita,

Matsuura,

Izawa

et al. 2024

ACS Sustainable Chem. Eng.

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“… 15 These limitations have restricted the development of solid ε-PL to a soft hydrogel 16 , 17 and a few other materials. 18 − 21 To overcome the poor moldability, we increased the apparent molecular weight of ε-PL by forming a molecular complex via ionic interactions with an anionic detergent 18 or a lignin derivative. 19 …”

Section: Introductionmentioning

confidence: 99%

“…The low molecular weight of ε-PL leads to poor moldability, although it is thermoplastic when dry and has a glass transition temperature of 88 °C and melting point of 173 °C . These limitations have restricted the development of solid ε-PL to a soft hydrogel , and a few other materials. − To overcome the poor moldability, we increased the apparent molecular weight of ε-PL by forming a molecular complex via ionic interactions with an anionic detergent or a lignin derivative …”

Section: Introductionmentioning

confidence: 99%

Bio-Based, Flexible, and Tough Material Derived from ε-Poly-l-lysine and Fructose via the Maillard Reaction

2020

Self Cite

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We report a bio-based, soft, elastic, and tough material prepared from a mixture of ε-poly- l -lysine (ε-PL) and d -fructose. The obtained complex was insoluble in water, whereas its ingredients had high water solubility. This complex was likely formed via Schiff base formation and subsequent rearrangement reactions, that is, the Maillard reaction, because the reaction occurred between reducing sugars and cationic polyelectrolytes having primary and secondary amino groups. The progress of the Maillard reaction was investigated by proton nuclear magnetic resonance spectroscopy and Fourier transform infrared spectroscopy. Mechanical properties of the complexes were evaluated by tensile testing, and the properties of the optimized complex [ε-PL/fructose = 60:40 (w/w), maximum stress = 27.9 MPa, strain at break = 46%, Young’s modulus = 741.6 MPa] resembled those of some petroleum-based plastics. Additionally, the ε-PL/fructose complex displayed antimicrobial activity against Bacillus subtilis . These ε-PL/fructose complexes have biological properties such as antimicrobial activity, low toxicity toward mammals, and biodegradability, which are attributable to the intrinsic nature of ε-PL, as well as enhanced mechanical properties and water resistance compared with pure ε-PL.

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“…For dispersions, they can be cast or poured into certain molds, followed by evaporation. The disadvantages of this method are the heterogeneity in particle size and coalescence, and the difficulty to control film thickness [132][133][134][135][136][137]. Except the previous mentioned extrusion, another way for processing PEC sediments is using compression with or without heat.…”

Section: Towards One-step Pec Film Formationmentioning

confidence: 99%

Single-step polyelectrolyte film formation by evaporation-induced complexation

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As discussed in the Preface and Introduction, plastic pollution is an issue that involves everyone. Scientifically, all possible routes should be explored to improve the current situation. PECs which are governed by electrostatic interactions have versatile functionalities and potential recyclability. This thesis aims to study a novel evaporative-based method to produce polyelectrolyte complex films, understand their properties, and explore their possible applications.Chapter 2 showcases the first successful evaporation-induced complexation of polyethylenimine (PEI) and poly(acrylic acid) (PAA). PEI is temporarily uncharged by adding ammonia to the solution and after casting, PEI gradually gets charged due to ammonia evaporation. With this single-step casting method, the final dry films have controlled thickness and composition. This specific PEI/PAA combination also gives the films a gas barrier functionality.Chapter 3 further moves on to another pair of polyelectrolytes: PEI and poly(4-styrenesulfonic acid) (PSS). Replacing weak PAA with strong PSS results in an increase of the strength of complexation. As a result, films are much more brittle. To confirm that this brittleness is due to the complexation rather than chain entanglements, PEI/NaPSS is studied as a comparison.Chapter 4 focuses on reducing the brittleness by studying different types of plasticizers, including salt, polyols, and amphiphilic ionic liquids. Successful plasticization can be achieved by selecting the suitable plasticizers and concentrations.Chapter 5 investigates the effects of different bases and cosolvents on film formation. The final film properties are examined to check whether the rate of complexation/drying has an impact.Finally, Chapter 6 discusses and summarizes the major findings of this work. Furthermore, suggestions about both fundamental research and applications are given.

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Moldable Material from ε-Poly-l-lysine and Lignosulfonate: Mechanical and Self-Healing Properties of a Bio-Based Polyelectrolyte Complex

Cited by 12 publications

References 35 publications

Melanin Upcycling: Creation of Polymeric Materials from Melanin Decomposition Products

Melanin Upcycling: Creation of Polymeric Materials from Melanin Decomposition Products

Bio-Based, Flexible, and Tough Material Derived from ε-Poly-l-lysine and Fructose via the Maillard Reaction

Single-step polyelectrolyte film formation by evaporation-induced complexation

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