Ring-Opening Polymerization of Hemoglobin.,Biomacromolecules

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Ring-Opening Polymerization of Hemoglobin.
Biomacromolecules ( IF 5.5 ) Pub Date : 2019-02-15 , DOI: 10.1021/acs.biomac.8b01789
Takashi Matsuhira ₁ , Keizo Yamamoto ₁ , Hiromi Sakai ₁

Affiliation

Hemoglobin (Hb), an oxygen-carrying protein, has an α2β2 tetrameric structure that dissociates reversibly into two αβ dimers (α2β2 ⇄ 2αβ). We synthesized a cyclic Hb-ring monomer with two β subunits bound through a 10 kDa polyethylene glycol (PEG) chain. The monomer induced ring-opening polymerization to produce a supramolecular polymer via intersubunit interaction of αβ dimers of an Hb molecule at the PEG terminals. Both the ring-closed monomer and the ring-opened supramolecular polymer were then fixed covalently by intramolecular cross-linking of two β subunits. Quantification of fixed products at various monomer concentrations revealed the equilibrium constant ( K), a ratio of propagation and depropagation rate constants, as 5.68 mM-1. The average degree of polymerization ([Formula: see text]) increased proportionally, concomitantly with the initial monomer concentration. Hb polymer with [Formula: see text] = 13.2 ( Mn = ca. 1 MDa) was obtained by cross-linking at 2.33 mM. Our novel strategy of ring-opening polymerization of Hb will eventually realize a highly aligned and efficiently polymerized Hb for creating artificial oxygen carriers for a clinical use.

中文翻译：

血红蛋白的开环聚合。

血红蛋白（Hb）是一种载氧蛋白，具有一个α2β2四聚体结构，该结构可逆地解离成两个αβ二聚体（α2β2⇄2αβ）。我们合成了具有通过10 kDa聚乙二醇（PEG）链结合的两个β亚基的环状Hb环单体。所述单体通过在PEG末端的Hb分子的αβ二聚体的亚基相互作用而诱导开环聚合以产生超分子聚合物。然后通过两个β亚基的分子内交联将闭环的单体和开环的超分子聚合物二者共价固定。固定产物在各种单体浓度下的定量显示平衡常数（K），即传播速率与去传播速率常数之比，为5.68 mM-1。平均聚合度（[公式：参见文字]）按比例增加，伴随着初始单体浓度。通过在2.33mM下交联获得[分子式：见正文] ＝ 13.2（Mn ＝约1MDa）的Hb聚合物。我们新的Hb开环聚合策略将最终实现高度排列和高效聚合的Hb，以创建用于临床的人造氧载体。

更新日期：2019-02-04

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