Dynamic-Covalent Macromolecular Stars with Boronic Ester Linkages
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作者:
Bapat, Abhijeet P.
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So Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USASo Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
Bapat, Abhijeet P.
[1
]
Roy, Debashish
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So Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USASo Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
Roy, Debashish
[1
]
Ray, Jacob G.
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Univ So Mississippi, Sch Polymers & High Performance Mat, Hattiesburg, MS 39406 USASo Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
Ray, Jacob G.
[3
]
Savin, Daniel A.
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Univ So Mississippi, Sch Polymers & High Performance Mat, Hattiesburg, MS 39406 USASo Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
Savin, Daniel A.
[3
]
Sumerlin, Brent S.
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So Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
So Methodist Univ, Ctr Drug Discovery Design & Delivery, Dallas, TX 75275 USASo Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
Sumerlin, Brent S.
[1
,2
]
机构:
[1] So Methodist Univ, Dept Chem, 3215 Daniel Ave, Dallas, TX 75275 USA
[2] So Methodist Univ, Ctr Drug Discovery Design & Delivery, Dallas, TX 75275 USA
[3] Univ So Mississippi, Sch Polymers & High Performance Mat, Hattiesburg, MS 39406 USA
Macromolecular stars containing reversible boronic ester linkages were prepared by an arm-first approach by reacting well-defined boronic acid-containing block copolymers with multifunctional 1,2/1,3-diols. Homopolymers of 3-acrylamidophenylboronic acid (APBA) formed macroscopic dynamic-covalent networks when cross-linked with multifunctional diols. On the other hand, adding the diol cross-linkers to block copolymers of poly(N,N-dimethylacrylamide (PDMA))b-poly(APBA) led to nanosized multiarm stars with boronic ester cores and PDMA coronas. The assembly of the stars under a variety of conditions was considered. The dynamic-covalent nature of the boronic ester cross-links allowed the stars to reconfigure their covalent structure in the presence of monofunctional diols that competed for bonding with the boronic acid component. Therefore, the stars could be induced to dissociate via competitive exchange reactions. The star formation-dissociation process was shown to be repeatable over multiple cycles.