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Enhanced Self-Assembly and Mechanical Properties of Cellulose-Based Triblock Copolymers: Comparisons with Amylose-Based Triblock Copolymers

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Title: Enhanced Self-Assembly and Mechanical Properties of Cellulose-Based Triblock Copolymers: Comparisons with Amylose-Based Triblock Copolymers
Authors: Katsuhara, Satoshi Browse this author
Takagi, Yasuko Browse this author
Sunagawa, Naoki Browse this author
Igarashi, Kiyohiko Browse this author
Yamamoto, Takuya Browse this author
Tajima, Kenji Browse this author →KAKEN DB
Isono, Takuya Browse this author
Satoh, Toshifumi Browse this author →KAKEN DB
Keywords: self-assembly
block copolymers
sustainable elastomers
Issue Date: 26-Jul-2021
Publisher: American Chemical Society
Journal Title: sustainable chemistry & engineering
Volume: 9
Issue: 29
Start Page: 9779
End Page: 9788
Publisher DOI: 10.1021/acssuschemeng.1c02180
Abstract: Herein, we compared the microphase-separation behavior and mechanical properties of cellulose- and amylose-based block copolymers (BCPs). Various cellooligosaccharide triacetate-b-poly(delta-decanolactone)-b-cellooligosaccharide triacetates (AcCel(n)-b-PDL-b-AcCel(n)s), which are cellulose-based ABA-type BCPs, with PDL molecular weights of approximately 5, 10, and 20 kg mol(-1) and PDL volume fractions of 0.65, 0.77, and 0.87, were synthesized from alpha,omega-diazido-end-functionalized PDLs and propargyl-end-functionalized cellooligosaccharide triacetates via click chemistry. We adopted the cellodextrin-phosphorylase-mediated oligomerization of alpha-D-glucose-1-phosphase in the presence of a propargyl-end-functionalized cellobiose primer to synthesize the functional cellooligosaccharide segment. The maltooligosaccharide triacetate-b-poly(delta-decanolactone)-b-maltooligosaccharide triacetate (AcMal(n)-b-PDL-b-AcMal(n)s) amylose counterparts were also synthesized in a similar manner. Small-angle X-ray scattering experiments and atomic force microscopy revealed that AcCel(n)-b-PDL-b-AcCel(n)s are more likely to microphase-separate into ordered nanostructures compared to AcMal(n)-b-PDL-b-AcMal(n)s, despite their comparable chemical compositions and molecular weights. Furthermore, AcCel(n)-b-PDL-b-AcCel(n)s exhibited significantly superior mechanical performance compared to their amylose counterparts under tensile testing, with Young's modulus and stress at break of AcCel(n)-b-PDL10k-b-AcCel(n) being 2.3 and 1.8 times higher, respectively, than those of AcMal(n)-b-PDL10k-b-AcMal(n). The enhanced microphase-separation and mechanical properties of AcCel(n)-b-PDL-b-AcCel(n)s were found to be attributable to the stiffness and crystalline nature of the AcCel(n) segments. These results demonstrate the advantages of using cellulose derivatives to synthesize novel biofunctional materials.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS sustainable chemistry & engineering, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Type: article (author version)
Appears in Collections:工学院・工学研究院 (Graduate School of Engineering / Faculty of Engineering) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 佐藤 敏文

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