Effect of degree of substitution on the microphase separation and mechanical properties of cellooligosaccharide acetate-based elastomers

Satoshi Katsuhara; Naoki Sunagawa; Kiyohiko Igarashi; Yutaka Takeuchi; Kenji Takahashi; Takuya Yamamoto; Feng Li; Kenji Tajima; Takuya Isono; Toshifumi Satoh

doi:10.1016/j.carbpol.2023.120976

Effect of degree of substitution on the microphase separation and mechanical properties of cellooligosaccharide acetate-based elastomers

Satoshi Katsuhara
, Naoki Sunagawa
, Kiyohiko Igarashi
, Yutaka Takeuchi
, Kenji Takahashi
, Takuya Yamamoto
, Feng Li
, Kenji Tajima^*
, Takuya Isono
, Toshifumi Satoh

^*Corresponding author for this work

Hokkaido University
University of Tokyo
Kanazawa University

Research output: Contribution to journal › Article › Scientific › peer-review

14 Citations (Scopus)

Abstract

Thermoplastic elastomers (TPEs) have long been used in a wide range of industries. However, most existing TPEs are petroleum-derived polymers. To realize environmentally benign alternatives to conventional TPEs, cellulose acetate is a promising TPE hard segment because of its sufficient mechanical properties, availability from renewable sources, and biodegradability in natural environments. Because the degree of substitution (DS) of cellulose acetate governs a range of physical properties, it is a useful parameter for designing novel cellulose acetate-based TPEs. In this study, we synthesized cellulose acetate-based ABA-type triblock copolymers (AcCel_x-b-PDL-b-AcCel_x) containing a celloologosaccharide acetate hard A segment (AcCel_x, where x is the DS; x = 3.0, 2.6, and 2.3) and a poly(δ-decanolactone) (PDL) soft B segment. Small-angle X-ray scattering showed that decreasing the DS of AcCel_x-b-PDL-b-AcCel_x resulted in the formation of a more ordered microphase-separated structure. Owing to the microphase separation of the hard cellulosic and soft PDL segments, all the AcCel_x-b-PDL-b-AcCel_x samples exhibited elastomer-like properties. Moreover, the decrease in DS improved toughness and suppressed stress relaxation. Furthermore, preliminary biodegradation tests in an aqueous environment revealed that the decrease in DS endowed AcCel_x-b-PDL-b-AcCel_x with greater biodegradability potential. This work demonstrates the usefulness of cellulose acetate-based TPEs as next-generation sustainable materials.

Original language	English
Article number	120976
Journal	Carbohydrate Polymers
Volume	316
DOIs	https://doi.org/10.1016/j.carbpol.2023.120976
Publication status	Published - 15 Sept 2023
MoE publication type	A1 Journal article-refereed

Funding

This work was supported by JSPS Grants-in-Aid for Scientific Research (B) (Nos. 19H02549 , 20H02792 , and 19H02769 ), the JSPS Fund for the Promotion of Joint International Research (B) (No. 21KK0096 ), the Japan Science and Technology Agency (JST) COI-NEXT Program (Grant Number JPMJPF2102 ), “Bio-organic Material Recycle System in Space” on MEXT Coordination Funds for Promoting AeroSpace Utilization (Grant Number JPJ000959 ), the Frontier Chemistry Center (Hokkaido University), the Photoexcitonix Project (Hokkaido University), the Creative Research Institute (Hokkaido University), the Project of Junior Scientist Promotion in Hokkaido University , the Iketani Science and Technology Foundation , the Asahi Glass Foundation , and Toyota Riken .

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 9 Industry, Innovation, and Infrastructure

Keywords

Biodegradability
Cellulose acetate
Mechanical properties
Microphase separation
Self-assembly
Thermoplastic elastomer

Access to Document

10.1016/j.carbpol.2023.120976

Cite this

@article{0fd41cfda2e34d4b8b865e38d846750a,

title = "Effect of degree of substitution on the microphase separation and mechanical properties of cellooligosaccharide acetate-based elastomers",

abstract = "Thermoplastic elastomers (TPEs) have long been used in a wide range of industries. However, most existing TPEs are petroleum-derived polymers. To realize environmentally benign alternatives to conventional TPEs, cellulose acetate is a promising TPE hard segment because of its sufficient mechanical properties, availability from renewable sources, and biodegradability in natural environments. Because the degree of substitution (DS) of cellulose acetate governs a range of physical properties, it is a useful parameter for designing novel cellulose acetate-based TPEs. In this study, we synthesized cellulose acetate-based ABA-type triblock copolymers (AcCelx-b-PDL-b-AcCelx) containing a celloologosaccharide acetate hard A segment (AcCelx, where x is the DS; x = 3.0, 2.6, and 2.3) and a poly(δ-decanolactone) (PDL) soft B segment. Small-angle X-ray scattering showed that decreasing the DS of AcCelx-b-PDL-b-AcCelx resulted in the formation of a more ordered microphase-separated structure. Owing to the microphase separation of the hard cellulosic and soft PDL segments, all the AcCelx-b-PDL-b-AcCelx samples exhibited elastomer-like properties. Moreover, the decrease in DS improved toughness and suppressed stress relaxation. Furthermore, preliminary biodegradation tests in an aqueous environment revealed that the decrease in DS endowed AcCelx-b-PDL-b-AcCelx with greater biodegradability potential. This work demonstrates the usefulness of cellulose acetate-based TPEs as next-generation sustainable materials.",

keywords = "Biodegradability, Cellulose acetate, Mechanical properties, Microphase separation, Self-assembly, Thermoplastic elastomer",

author = "Satoshi Katsuhara and Naoki Sunagawa and Kiyohiko Igarashi and Yutaka Takeuchi and Kenji Takahashi and Takuya Yamamoto and Feng Li and Kenji Tajima and Takuya Isono and Toshifumi Satoh",

note = "Funding Information: This work was supported by JSPS Grants-in-Aid for Scientific Research (B) (Nos. 19H02549 , 20H02792 , and 19H02769 ), the JSPS Fund for the Promotion of Joint International Research (B) (No. 21KK0096 ), the Japan Science and Technology Agency (JST) COI-NEXT Program (Grant Number JPMJPF2102 ), “Bio-organic Material Recycle System in Space” on MEXT Coordination Funds for Promoting AeroSpace Utilization (Grant Number JPJ000959 ), the Frontier Chemistry Center (Hokkaido University), the Photoexcitonix Project (Hokkaido University), the Creative Research Institute (Hokkaido University), the Project of Junior Scientist Promotion in Hokkaido University , the Iketani Science and Technology Foundation , the Asahi Glass Foundation , and Toyota Riken . Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

year = "2023",

month = sep,

day = "15",

doi = "10.1016/j.carbpol.2023.120976",

language = "English",

volume = "316",

journal = "Carbohydrate Polymers",

issn = "0144-8617",

publisher = "Elsevier",

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TY - JOUR

T1 - Effect of degree of substitution on the microphase separation and mechanical properties of cellooligosaccharide acetate-based elastomers

AU - Katsuhara, Satoshi

AU - Sunagawa, Naoki

AU - Igarashi, Kiyohiko

AU - Takeuchi, Yutaka

AU - Takahashi, Kenji

AU - Yamamoto, Takuya

AU - Li, Feng

AU - Tajima, Kenji

AU - Isono, Takuya

AU - Satoh, Toshifumi

N1 - Funding Information: This work was supported by JSPS Grants-in-Aid for Scientific Research (B) (Nos. 19H02549 , 20H02792 , and 19H02769 ), the JSPS Fund for the Promotion of Joint International Research (B) (No. 21KK0096 ), the Japan Science and Technology Agency (JST) COI-NEXT Program (Grant Number JPMJPF2102 ), “Bio-organic Material Recycle System in Space” on MEXT Coordination Funds for Promoting AeroSpace Utilization (Grant Number JPJ000959 ), the Frontier Chemistry Center (Hokkaido University), the Photoexcitonix Project (Hokkaido University), the Creative Research Institute (Hokkaido University), the Project of Junior Scientist Promotion in Hokkaido University , the Iketani Science and Technology Foundation , the Asahi Glass Foundation , and Toyota Riken . Publisher Copyright: © 2023 Elsevier Ltd

PY - 2023/9/15

Y1 - 2023/9/15

N2 - Thermoplastic elastomers (TPEs) have long been used in a wide range of industries. However, most existing TPEs are petroleum-derived polymers. To realize environmentally benign alternatives to conventional TPEs, cellulose acetate is a promising TPE hard segment because of its sufficient mechanical properties, availability from renewable sources, and biodegradability in natural environments. Because the degree of substitution (DS) of cellulose acetate governs a range of physical properties, it is a useful parameter for designing novel cellulose acetate-based TPEs. In this study, we synthesized cellulose acetate-based ABA-type triblock copolymers (AcCelx-b-PDL-b-AcCelx) containing a celloologosaccharide acetate hard A segment (AcCelx, where x is the DS; x = 3.0, 2.6, and 2.3) and a poly(δ-decanolactone) (PDL) soft B segment. Small-angle X-ray scattering showed that decreasing the DS of AcCelx-b-PDL-b-AcCelx resulted in the formation of a more ordered microphase-separated structure. Owing to the microphase separation of the hard cellulosic and soft PDL segments, all the AcCelx-b-PDL-b-AcCelx samples exhibited elastomer-like properties. Moreover, the decrease in DS improved toughness and suppressed stress relaxation. Furthermore, preliminary biodegradation tests in an aqueous environment revealed that the decrease in DS endowed AcCelx-b-PDL-b-AcCelx with greater biodegradability potential. This work demonstrates the usefulness of cellulose acetate-based TPEs as next-generation sustainable materials.

AB - Thermoplastic elastomers (TPEs) have long been used in a wide range of industries. However, most existing TPEs are petroleum-derived polymers. To realize environmentally benign alternatives to conventional TPEs, cellulose acetate is a promising TPE hard segment because of its sufficient mechanical properties, availability from renewable sources, and biodegradability in natural environments. Because the degree of substitution (DS) of cellulose acetate governs a range of physical properties, it is a useful parameter for designing novel cellulose acetate-based TPEs. In this study, we synthesized cellulose acetate-based ABA-type triblock copolymers (AcCelx-b-PDL-b-AcCelx) containing a celloologosaccharide acetate hard A segment (AcCelx, where x is the DS; x = 3.0, 2.6, and 2.3) and a poly(δ-decanolactone) (PDL) soft B segment. Small-angle X-ray scattering showed that decreasing the DS of AcCelx-b-PDL-b-AcCelx resulted in the formation of a more ordered microphase-separated structure. Owing to the microphase separation of the hard cellulosic and soft PDL segments, all the AcCelx-b-PDL-b-AcCelx samples exhibited elastomer-like properties. Moreover, the decrease in DS improved toughness and suppressed stress relaxation. Furthermore, preliminary biodegradation tests in an aqueous environment revealed that the decrease in DS endowed AcCelx-b-PDL-b-AcCelx with greater biodegradability potential. This work demonstrates the usefulness of cellulose acetate-based TPEs as next-generation sustainable materials.

KW - Biodegradability

KW - Cellulose acetate

KW - Mechanical properties

KW - Microphase separation

KW - Self-assembly

KW - Thermoplastic elastomer

UR - https://www.scopus.com/pages/publications/85160850531

U2 - 10.1016/j.carbpol.2023.120976

DO - 10.1016/j.carbpol.2023.120976

M3 - Article

AN - SCOPUS:85160850531

SN - 0144-8617

VL - 316

JO - Carbohydrate Polymers

JF - Carbohydrate Polymers

M1 - 120976

ER -

Effect of degree of substitution on the microphase separation and mechanical properties of cellooligosaccharide acetate-based elastomers

Abstract

Funding

UN SDGs

Keywords

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