Enzymatic Polymerization of Poly(glycerol-1,8-octanediol-sebacate): Versatile Poly(glycerol sebacate) Analogues that Form Monocomponent Biodegradable Fiber Scaffolds.,Biomacromolecules

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Enzymatic Polymerization of Poly(glycerol-1,8-octanediol-sebacate): Versatile Poly(glycerol sebacate) Analogues that Form Monocomponent Biodegradable Fiber Scaffolds.
Biomacromolecules ( IF 5.5 ) Pub Date : 2020-06-19 , DOI: 10.1021/acs.biomac.0c00641
Kening Lang ₁ , Somdatta Bhattacharya ₂ , Zhuoyuan Ning _{1,

3} , Regina J Sánchez-Leija ₁ , Michael T K Bramson ₄ , Robert Centore ₁ , David T Corr ₄ , Robert J Linhardt _{1,

2,

4,

5} , Richard A Gross _{1,

2,

4,

5}

Affiliation

A family of poly(glycerol sebacate) (PGS) analogues were synthesized by Candida antarctica lipase B (CALB) catalysis to tailor biomaterial properties. Different fractions of glycerol (G) units in PGS were replaced by 1,8-octanediol (O) units. Poly(glycerol-1,8-octanediol-sebacate), PGOS, synthesized by CALB catalysis with a 1:3 molar ratio of G to O units has M_n and M_w values of 9500 and 92,000, respectively. PGS undergoes fiber fusion during electrospinning, and cross-linked PGS rapidly resorbs when implanted. By decreasing the molar ratio of glycerol-to-octanediol from 1:1 to 1:4, the peak melting temperature (T_m) increased from 27 to 47 °C. PGOS with 1:3 G to O units was electrospun into nanofibers without the need for a second component. The copolymer is semicrystalline and, when cross-linked, undergoes slow in vitro mass loss (3.5 ± 1.0% in 31 days) at pH 7.4 and 37 °C. Furthermore, PGOS cross-linked films have an elastic modulus of 106.1 ± 18.6 MPa, which is more than 100 times that of cross-linked PGS. New PGOS polymers showed tunable molecular weights, better thermal properties, and excellent electrospinnability. This work expanded PGS analogues’ function, making these suitable biodegradable polymers for various biomedical applications.

中文翻译：

聚（1,8-辛二醇-癸二酸甘油酯）的酶促聚合反应：形成单组分可生物降解纤维支架的通用聚（癸二酸甘油酯）类似物。

通过南极假丝酵母脂肪酶B（CALB）催化合成了聚癸二酸甘油酯（PGS）类似物家族，以调整生物材料的特性。PGS中不同比例的甘油（G）单元被1,8-辛二醇（O）单元取代。通过CALB催化以1∶3的G与O单元的摩尔比合成的聚（1，8-辛二醇-癸二酸甘油酯）PGOS的M _n和M _w分别为9500和92,000。PGS在静电纺丝过程中会发生纤维融合，而交联的PGS在植入后会迅速吸收。通过将甘油与辛二醇的摩尔比从1：1降低至1：4，可达到峰值熔融温度（T _m）从27°C升至47°C。将具有1：3 G到O单位的PGOS静电纺成纳米纤维，而无需第二种成分。该共聚物是半结晶的，当交联时，在pH 7.4和37°C下，其体外质量损失缓慢（31天为3.5±1.0％）。此外，PGOS交联膜的弹性模量为106.1±18.6 MPa，是交联PGS的100倍以上。新型PGOS聚合物显示出可调节的分子量，更好的热性能和出色的电纺性。这项工作扩展了PGS类似物的功能，使这些适合生物降解的聚合物适用于各种生物医学应用。

更新日期：2020-08-10

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