Alginate-based diblock polymers: preparation, characterization and Ca-induced self-assembly
Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers. Alginates are natural polysaccharides widely used as biomaterials. Functional properties depend on the content and distributio...
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Veröffentlicht in: | Polymer chemistry 2021-10, Vol.12 (38), p.5412-5425 |
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creator | Solberg, Amalie Mo, Ingrid V Aachmann, Finn L Schatz, Christophe Christensen, Bjørn E |
description | Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers. Alginates are natural polysaccharides widely used as biomaterials. Functional properties depend on the content and distribution of the two 4-linked monomers (β-
d
-mannuronate (M) and α-
l
-guluronate (G)). Blocks of
l
-guluronate (G
n
) are responsible for cooperative binding of calcium ions and hydrogel formation. Incorporation of such blocks in block polysaccharide copolymers would represent a new class of engineered, Ca-sensitive biomacromolecules. Dioxyamines and dihydrazides have recently been shown to be well suited for preparation of block polysaccharide structures. Here we first show that when applied to alginate blocks (G
n
and M
n
) the two types are both very reactive, but the detailed distribution of acyclic (
E
)- and (
Z
)-forms and cyclic
N
-pyranosides, reaction kinetics, conjugate stability, and the rate of Schiff base reduction with α-picoline borane differ considerably, also compared to other polysaccharides. Hence, alginate specific protocols were developed. The linkers introduce a highly flexible joint in otherwise semiflexible G
n
-based diblocks. This was demonstrated by SEC-MALS using a symmetrical G
n
-
b
-G
n
diblock, which in solution can best be described according to a broken rod model. Ca-Induced self-assembly of G
n
-
b
-dextran diblocks was studied by dynamic light scattering, demonstrating that well defined nanoparticles could be prepared for certain combinations of chain lengths. Taken together, this approach provides a new class of engineered, stimuli-responsive block polysaccharide copolymers solely based on natural resources.
Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers. |
doi_str_mv | 10.1039/d1py00727k |
format | Article |
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d
-mannuronate (M) and α-
l
-guluronate (G)). Blocks of
l
-guluronate (G
n
) are responsible for cooperative binding of calcium ions and hydrogel formation. Incorporation of such blocks in block polysaccharide copolymers would represent a new class of engineered, Ca-sensitive biomacromolecules. Dioxyamines and dihydrazides have recently been shown to be well suited for preparation of block polysaccharide structures. Here we first show that when applied to alginate blocks (G
n
and M
n
) the two types are both very reactive, but the detailed distribution of acyclic (
E
)- and (
Z
)-forms and cyclic
N
-pyranosides, reaction kinetics, conjugate stability, and the rate of Schiff base reduction with α-picoline borane differ considerably, also compared to other polysaccharides. Hence, alginate specific protocols were developed. The linkers introduce a highly flexible joint in otherwise semiflexible G
n
-based diblocks. This was demonstrated by SEC-MALS using a symmetrical G
n
-
b
-G
n
diblock, which in solution can best be described according to a broken rod model. Ca-Induced self-assembly of G
n
-
b
-dextran diblocks was studied by dynamic light scattering, demonstrating that well defined nanoparticles could be prepared for certain combinations of chain lengths. Taken together, this approach provides a new class of engineered, stimuli-responsive block polysaccharide copolymers solely based on natural resources.
Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers.</description><identifier>ISSN: 1759-9954</identifier><identifier>EISSN: 1759-9962</identifier><identifier>DOI: 10.1039/d1py00727k</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Alginates ; Biomedical materials ; Block copolymers ; Calcium ions ; Chemical Sciences ; Dextrans ; Hydrogels ; Imines ; Nanoparticles ; Natural resources ; Photon correlation spectroscopy ; Polymer chemistry ; Polymers ; Polysaccharides ; Reaction kinetics ; Renewable resources ; Self-assembly ; Stimuli</subject><ispartof>Polymer chemistry, 2021-10, Vol.12 (38), p.5412-5425</ispartof><rights>Copyright Royal Society of Chemistry 2021</rights><rights>Attribution - NonCommercial - ShareAlike</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c351t-f276a33cbaa88100797f00b846fd756c05a06b03b05c2ccb20e840d944def73</citedby><cites>FETCH-LOGICAL-c351t-f276a33cbaa88100797f00b846fd756c05a06b03b05c2ccb20e840d944def73</cites><orcidid>0000-0003-1613-4663 ; 0000-0002-1135-9815</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,780,784,885,27924,27925</link.rule.ids><backlink>$$Uhttps://hal.science/hal-03511278$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Solberg, Amalie</creatorcontrib><creatorcontrib>Mo, Ingrid V</creatorcontrib><creatorcontrib>Aachmann, Finn L</creatorcontrib><creatorcontrib>Schatz, Christophe</creatorcontrib><creatorcontrib>Christensen, Bjørn E</creatorcontrib><title>Alginate-based diblock polymers: preparation, characterization and Ca-induced self-assembly</title><title>Polymer chemistry</title><description>Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers. Alginates are natural polysaccharides widely used as biomaterials. Functional properties depend on the content and distribution of the two 4-linked monomers (β-
d
-mannuronate (M) and α-
l
-guluronate (G)). Blocks of
l
-guluronate (G
n
) are responsible for cooperative binding of calcium ions and hydrogel formation. Incorporation of such blocks in block polysaccharide copolymers would represent a new class of engineered, Ca-sensitive biomacromolecules. Dioxyamines and dihydrazides have recently been shown to be well suited for preparation of block polysaccharide structures. Here we first show that when applied to alginate blocks (G
n
and M
n
) the two types are both very reactive, but the detailed distribution of acyclic (
E
)- and (
Z
)-forms and cyclic
N
-pyranosides, reaction kinetics, conjugate stability, and the rate of Schiff base reduction with α-picoline borane differ considerably, also compared to other polysaccharides. Hence, alginate specific protocols were developed. The linkers introduce a highly flexible joint in otherwise semiflexible G
n
-based diblocks. This was demonstrated by SEC-MALS using a symmetrical G
n
-
b
-G
n
diblock, which in solution can best be described according to a broken rod model. Ca-Induced self-assembly of G
n
-
b
-dextran diblocks was studied by dynamic light scattering, demonstrating that well defined nanoparticles could be prepared for certain combinations of chain lengths. Taken together, this approach provides a new class of engineered, stimuli-responsive block polysaccharide copolymers solely based on natural resources.
Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers.</description><subject>Alginates</subject><subject>Biomedical materials</subject><subject>Block copolymers</subject><subject>Calcium ions</subject><subject>Chemical Sciences</subject><subject>Dextrans</subject><subject>Hydrogels</subject><subject>Imines</subject><subject>Nanoparticles</subject><subject>Natural resources</subject><subject>Photon correlation spectroscopy</subject><subject>Polymer chemistry</subject><subject>Polymers</subject><subject>Polysaccharides</subject><subject>Reaction kinetics</subject><subject>Renewable resources</subject><subject>Self-assembly</subject><subject>Stimuli</subject><issn>1759-9954</issn><issn>1759-9962</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNpFkUtLw0AQxxdRsGgv3oWAJ8Xo7CPZxFupj4oFBb2Ih2VfsWnTJO6mQvz0blupc5nhz2_eCJ1guMJA82uD2x6AE77YQwPMkzzO85Ts7-KEHaKh93MIRjEjNB2gj1H1Wdays7GS3prIlKpq9CJqm6pfWudvotbZVjrZlU19GelZCHVnXfmzUSJZm2gs47I2Kx3Sva2KWHpvl6rqj9FBIStvh3_-CL3e372NJ_H0-eFxPJrGmia4iwvCU0mpVlJmGQ4L5LwAUBlLC8OTVEMiIVVAFSSaaK0I2IyByRkztuD0CJ1vq85kJVpXLqXrRSNLMRlNxVqD0AUTnn3jwJ5t2dY1XyvrOzFvVq4OwwmS8BwYIYQF6mJLadd472yxK4tBrC8tbvHL--bSTwE-3cLO6x33_wn6C5-jegk</recordid><startdate>20211005</startdate><enddate>20211005</enddate><creator>Solberg, Amalie</creator><creator>Mo, Ingrid V</creator><creator>Aachmann, Finn L</creator><creator>Schatz, Christophe</creator><creator>Christensen, Bjørn E</creator><general>Royal Society of Chemistry</general><general>Royal Society of Chemistry - RSC</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8FD</scope><scope>JG9</scope><scope>1XC</scope><scope>VOOES</scope><orcidid>https://orcid.org/0000-0003-1613-4663</orcidid><orcidid>https://orcid.org/0000-0002-1135-9815</orcidid></search><sort><creationdate>20211005</creationdate><title>Alginate-based diblock polymers: preparation, characterization and Ca-induced self-assembly</title><author>Solberg, Amalie ; Mo, Ingrid V ; Aachmann, Finn L ; Schatz, Christophe ; Christensen, Bjørn E</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c351t-f276a33cbaa88100797f00b846fd756c05a06b03b05c2ccb20e840d944def73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Alginates</topic><topic>Biomedical materials</topic><topic>Block copolymers</topic><topic>Calcium ions</topic><topic>Chemical Sciences</topic><topic>Dextrans</topic><topic>Hydrogels</topic><topic>Imines</topic><topic>Nanoparticles</topic><topic>Natural resources</topic><topic>Photon correlation spectroscopy</topic><topic>Polymer chemistry</topic><topic>Polymers</topic><topic>Polysaccharides</topic><topic>Reaction kinetics</topic><topic>Renewable resources</topic><topic>Self-assembly</topic><topic>Stimuli</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Solberg, Amalie</creatorcontrib><creatorcontrib>Mo, Ingrid V</creatorcontrib><creatorcontrib>Aachmann, Finn L</creatorcontrib><creatorcontrib>Schatz, Christophe</creatorcontrib><creatorcontrib>Christensen, Bjørn E</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Hyper Article en Ligne (HAL)</collection><collection>Hyper Article en Ligne (HAL) (Open Access)</collection><jtitle>Polymer chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Solberg, Amalie</au><au>Mo, Ingrid V</au><au>Aachmann, Finn L</au><au>Schatz, Christophe</au><au>Christensen, Bjørn E</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Alginate-based diblock polymers: preparation, characterization and Ca-induced self-assembly</atitle><jtitle>Polymer chemistry</jtitle><date>2021-10-05</date><risdate>2021</risdate><volume>12</volume><issue>38</issue><spage>5412</spage><epage>5425</epage><pages>5412-5425</pages><issn>1759-9954</issn><eissn>1759-9962</eissn><abstract>Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers. Alginates are natural polysaccharides widely used as biomaterials. Functional properties depend on the content and distribution of the two 4-linked monomers (β-
d
-mannuronate (M) and α-
l
-guluronate (G)). Blocks of
l
-guluronate (G
n
) are responsible for cooperative binding of calcium ions and hydrogel formation. Incorporation of such blocks in block polysaccharide copolymers would represent a new class of engineered, Ca-sensitive biomacromolecules. Dioxyamines and dihydrazides have recently been shown to be well suited for preparation of block polysaccharide structures. Here we first show that when applied to alginate blocks (G
n
and M
n
) the two types are both very reactive, but the detailed distribution of acyclic (
E
)- and (
Z
)-forms and cyclic
N
-pyranosides, reaction kinetics, conjugate stability, and the rate of Schiff base reduction with α-picoline borane differ considerably, also compared to other polysaccharides. Hence, alginate specific protocols were developed. The linkers introduce a highly flexible joint in otherwise semiflexible G
n
-based diblocks. This was demonstrated by SEC-MALS using a symmetrical G
n
-
b
-G
n
diblock, which in solution can best be described according to a broken rod model. Ca-Induced self-assembly of G
n
-
b
-dextran diblocks was studied by dynamic light scattering, demonstrating that well defined nanoparticles could be prepared for certain combinations of chain lengths. Taken together, this approach provides a new class of engineered, stimuli-responsive block polysaccharide copolymers solely based on natural resources.
Renewable resources can provide a range of different polysaccharide blocks that can be used to prepare new types of stimuli-responsive polysaccharide-based block copolymers.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d1py00727k</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0003-1613-4663</orcidid><orcidid>https://orcid.org/0000-0002-1135-9815</orcidid><oa>free_for_read</oa></addata></record> |
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source | Royal Society Of Chemistry Journals |
subjects | Alginates Biomedical materials Block copolymers Calcium ions Chemical Sciences Dextrans Hydrogels Imines Nanoparticles Natural resources Photon correlation spectroscopy Polymer chemistry Polymers Polysaccharides Reaction kinetics Renewable resources Self-assembly Stimuli |
title | Alginate-based diblock polymers: preparation, characterization and Ca-induced self-assembly |
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