Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants
In recent years, there has been considerable research into functional materials inspired by living things. Much attention has been paid to the development of adhesive materials that mimic the adhesive proteins secreted by a mussel’s foot. These mussel-inspired materials have superior adhesiveness to...
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MDPI AG
2022-12-01
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| Series: | Materials |
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| Online Access: | https://www.mdpi.com/1996-1944/16/1/266 |
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| author | Takehiro Fujita Masami Shuta Mika Mano Shinnosuke Matsumoto Atsushi Nagasawa Akihiro Yamada Masanobu Naito |
| author_facet | Takehiro Fujita Masami Shuta Mika Mano Shinnosuke Matsumoto Atsushi Nagasawa Akihiro Yamada Masanobu Naito |
| author_sort | Takehiro Fujita |
| collection | DOAJ |
| description | In recent years, there has been considerable research into functional materials inspired by living things. Much attention has been paid to the development of adhesive materials that mimic the adhesive proteins secreted by a mussel’s foot. These mussel-inspired materials have superior adhesiveness to various adherents owing to the non-covalent interactions of their polyphenolic moieties, e.g., hydrogen bonding, electrostatic interactions, and even hydrophobic interactions. Various factors significantly affect the adhesiveness of mussel-inspired polymers, such as the molecular weight, cross-linking density, and composition ratio of the components, as well as the chemical structure of the polyphenolic adhesive moieties, such as <span style="font-variant: small-caps;">l</span>-3,4-dihydroxyphenylalanine (<span style="font-variant: small-caps;">l</span>-Dopa). However, the contributions of the position and distribution of the adhesive moiety in mussel-inspired polymers are often underestimated. In the present study, we prepared a series of mussel-inspired alkyl methacrylate copolymers by controlling the position and distribution of the adhesive moiety, which are known as “forced gradient copolymers”. We used a newly designed gallic-acid-bearing methacrylate (GMA) as the polyphenolic adhesive moiety and copolymerized it with 2-ethylhexyl methacrylate (EHMA). The resulting forced gradient adhesive copolymer of GMA and EHMA (poly(GMA-<i>co</i>-EHMA), Poly<b>1</b>) was subjected to adhesion and dispersion tests with an aluminum substrate and a BaTiO<sub>3</sub> nanoparticle in organic solvents, respectively. In particular, this study aims to clarify how the monomer position and distribution of the adhesive moiety in the mussel-inspired polymer affect its adhesion and dispersion behavior on a flat metal oxide surface and spherical inorganic oxide surfaces of several tens of nanometers in diameter, respectively. Here, forced gradient copolymer Poly<b>1</b> consisted of a homopolymer moiety of EHMA (Poly<b>3</b>) and a random copolymer moiety of EHMA and GMA (Poly<b>4</b>). The composition ratio of GMA and the molecular weight were kept constant among the Poly<b>1</b> series. Simultaneous control of the molecular lengths of Poly<b>3</b> and Poly<b>4 </b> allowed us to discuss the effects on the distribution of GMA in Poly<b>1</b>. Poly<b>1</b> exhibited apparent distribution dependency with regard to the adhesiveness and the dispersibility of BaTiO<sub>3</sub>. Poly<b>1</b> showed the highest adhesion strength when the composition ratio of GMA was approximately 9 mol% in the portion of the Poly<b>4</b> segment. In contrast, the block copolymer consisting of the Poly<b>3</b> segment and Poly<b>4</b> segment with only adhesive moiety <b>1</b> showed the lowest viscosity for dispersion of BaTiO<sub>3</sub> nanoparticles. These results indicate that copolymers with mussel-inspired adhesive motifs require the proper design of the monomer position and distribution in Poly<b>1</b> according to the shape and characteristics of the adherend to maximize their functionality. This research will facilitate the rational design of bio-inspired adhesive materials derived from plants that outperform natural materials, and it will eventually contribute to a sustainable circular economy. |
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| format | Article |
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| institution | Directory Open Access Journal |
| issn | 1996-1944 |
| language | English |
| last_indexed | 2024-03-11T09:56:27Z |
| publishDate | 2022-12-01 |
| publisher | MDPI AG |
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| series | Materials |
| spelling | doaj.art-ee867018fde641f39e000248507df65b2023-11-16T15:49:20ZengMDPI AGMaterials1996-19442022-12-0116126610.3390/ma16010266Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and DispersantsTakehiro Fujita0Masami Shuta1Mika Mano2Shinnosuke Matsumoto3Atsushi Nagasawa4Akihiro Yamada5Masanobu Naito6Data-Driven Polymer Design Group, Research and Services Division of Materials Data and Integrated System (MaDIS), National Institute for Materials Science (NIMS), Ibaraki 305-0047, JapanData-Driven Polymer Design Group, Research and Services Division of Materials Data and Integrated System (MaDIS), National Institute for Materials Science (NIMS), Ibaraki 305-0047, JapanData-Driven Polymer Design Group, Research and Services Division of Materials Data and Integrated System (MaDIS), National Institute for Materials Science (NIMS), Ibaraki 305-0047, JapanOleo & Speciality Chemicals Research Lab., NOF Corporation, Hyogo 660-0095, JapanOleo & Speciality Chemicals Research Lab., NOF Corporation, Hyogo 660-0095, JapanOleo & Speciality Chemicals Research Lab., NOF Corporation, Hyogo 660-0095, JapanData-Driven Polymer Design Group, Research and Services Division of Materials Data and Integrated System (MaDIS), National Institute for Materials Science (NIMS), Ibaraki 305-0047, JapanIn recent years, there has been considerable research into functional materials inspired by living things. Much attention has been paid to the development of adhesive materials that mimic the adhesive proteins secreted by a mussel’s foot. These mussel-inspired materials have superior adhesiveness to various adherents owing to the non-covalent interactions of their polyphenolic moieties, e.g., hydrogen bonding, electrostatic interactions, and even hydrophobic interactions. Various factors significantly affect the adhesiveness of mussel-inspired polymers, such as the molecular weight, cross-linking density, and composition ratio of the components, as well as the chemical structure of the polyphenolic adhesive moieties, such as <span style="font-variant: small-caps;">l</span>-3,4-dihydroxyphenylalanine (<span style="font-variant: small-caps;">l</span>-Dopa). However, the contributions of the position and distribution of the adhesive moiety in mussel-inspired polymers are often underestimated. In the present study, we prepared a series of mussel-inspired alkyl methacrylate copolymers by controlling the position and distribution of the adhesive moiety, which are known as “forced gradient copolymers”. We used a newly designed gallic-acid-bearing methacrylate (GMA) as the polyphenolic adhesive moiety and copolymerized it with 2-ethylhexyl methacrylate (EHMA). The resulting forced gradient adhesive copolymer of GMA and EHMA (poly(GMA-<i>co</i>-EHMA), Poly<b>1</b>) was subjected to adhesion and dispersion tests with an aluminum substrate and a BaTiO<sub>3</sub> nanoparticle in organic solvents, respectively. In particular, this study aims to clarify how the monomer position and distribution of the adhesive moiety in the mussel-inspired polymer affect its adhesion and dispersion behavior on a flat metal oxide surface and spherical inorganic oxide surfaces of several tens of nanometers in diameter, respectively. Here, forced gradient copolymer Poly<b>1</b> consisted of a homopolymer moiety of EHMA (Poly<b>3</b>) and a random copolymer moiety of EHMA and GMA (Poly<b>4</b>). The composition ratio of GMA and the molecular weight were kept constant among the Poly<b>1</b> series. Simultaneous control of the molecular lengths of Poly<b>3</b> and Poly<b>4 </b> allowed us to discuss the effects on the distribution of GMA in Poly<b>1</b>. Poly<b>1</b> exhibited apparent distribution dependency with regard to the adhesiveness and the dispersibility of BaTiO<sub>3</sub>. Poly<b>1</b> showed the highest adhesion strength when the composition ratio of GMA was approximately 9 mol% in the portion of the Poly<b>4</b> segment. In contrast, the block copolymer consisting of the Poly<b>3</b> segment and Poly<b>4</b> segment with only adhesive moiety <b>1</b> showed the lowest viscosity for dispersion of BaTiO<sub>3</sub> nanoparticles. These results indicate that copolymers with mussel-inspired adhesive motifs require the proper design of the monomer position and distribution in Poly<b>1</b> according to the shape and characteristics of the adherend to maximize their functionality. This research will facilitate the rational design of bio-inspired adhesive materials derived from plants that outperform natural materials, and it will eventually contribute to a sustainable circular economy.https://www.mdpi.com/1996-1944/16/1/266mussel-inspired polymeradhesivedispersantforced gradient polymer<span style="font-variant: small-caps">l</span>-3,4-dihydroxyphenylalaninedopamine |
| spellingShingle | Takehiro Fujita Masami Shuta Mika Mano Shinnosuke Matsumoto Atsushi Nagasawa Akihiro Yamada Masanobu Naito Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants Materials mussel-inspired polymer adhesive dispersant forced gradient polymer <span style="font-variant: small-caps">l</span>-3,4-dihydroxyphenylalanine dopamine |
| title | Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants |
| title_full | Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants |
| title_fullStr | Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants |
| title_full_unstemmed | Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants |
| title_short | Forced Gradient Copolymer for Rational Design of Mussel-Inspired Adhesives and Dispersants |
| title_sort | forced gradient copolymer for rational design of mussel inspired adhesives and dispersants |
| topic | mussel-inspired polymer adhesive dispersant forced gradient polymer <span style="font-variant: small-caps">l</span>-3,4-dihydroxyphenylalanine dopamine |
| url | https://www.mdpi.com/1996-1944/16/1/266 |
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