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引入血红蛋白的超分子聚合物水凝胶的粘弹性随pH值、温度和氧分压的变化

Change in Viscoelasticity of the Hemoglobin-Introduced Supramolecular Polymer Hydrogel in Response to pH, Temperature, and Oxygen Partial Pressure.

作者信息

Matsuhira Takashi, Sakai Hiromi

机构信息

Department of Chemistry, Nara Medical University, 88 Shijo-cho, Kashihara 634-0813, Japan.

出版信息

Biomacromolecules. 2025 Aug 11;26(8):5212-5223. doi: 10.1021/acs.biomac.5c00669. Epub 2025 Jul 29.

Abstract

Hemoglobin (Hb) compartmentalized within red blood cells plays a key role in respiration by reversible oxygen (O) binding at the site of ferrous heme iron. The stable αβ tetrameric quaternary structure of Hb reversibly dissociates into two αβ dimers (αβ ⇌ 2αβ). The αβ structure stability depends on pH and temperature, and on the state of heme, such as iron valence, ligands, and O release. For this work, we synthesized a supramolecular polymer hydrogel by conjugating the β-subunits of Hb with four-armed 40 kDa PEG. The resulting gel has physical cross-links via the association of Hb subunits. It therefore undergoes changes in viscoelasticity upon multiple external stimuli, including changes in pH, temperature, and the O partial pressure (pO). It is noteworthy that the characteristic relaxation time τ and the zero-shear viscosity η both increase ca. 100-fold in response to O dissociation occurring with lower pO. This paper is the first to present a synthetic hydrogel that can switch the viscoelasticity by binding and releasing O, demonstrating this "respirable" gel as a promising O-responsive smart material.

摘要

红细胞内的血红蛋白(Hb)通过亚铁血红素铁部位的可逆氧(O)结合在呼吸中起关键作用。Hb稳定的αβ四聚体四级结构可逆地解离成两个αβ二聚体(αβ⇌2αβ)。αβ结构的稳定性取决于pH值、温度以及血红素的状态,如铁价态、配体和氧释放情况。在本研究中,我们通过将Hb的β亚基与四臂40 kDa聚乙二醇(PEG)共轭合成了一种超分子聚合物水凝胶。所得凝胶通过Hb亚基的缔合形成物理交联。因此,它在多种外部刺激下,包括pH值、温度和氧分压(pO)的变化,会发生粘弹性变化。值得注意的是,随着较低pO下发生的氧解离,特征弛豫时间τ和零剪切粘度η均增加约100倍。本文首次报道了一种可通过结合和释放氧来切换粘弹性的合成水凝胶,证明这种“可呼吸”凝胶是一种有前景的氧响应智能材料。

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