Revealing the Relationship between the Biocompatibility and the Bound Water of Poly(ethylene glycol) by Single-molecule Force Spectroscopy

Jun Xu; Nan-pu Cao; Yao-xin Xiao; Zhong-long Luo; Yu Bao; Shu-xun Cui

doi:10.11777/j.issn1000-3304.2019.19219

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Revealing the Relationship between the Biocompatibility and the Bound Water of Poly(ethylene glycol) by Single-molecule Force Spectroscopy

更新时间：2021-01-26

- Revealing the Relationship between the Biocompatibility and the Bound Water of Poly(ethylene glycol) by Single-molecule Force Spectroscopy
  增强出版
- Acta Polymerica Sinica Vol. 51, Issue 7, Pages: 754-761(2020)
- 作者机构：
  
  材料先进技术教育部重点实验室西南交通大学　成都 610031
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2019.19219
  CLC：
- Published：2020-7，
  
  Published Online：19 May 2020，
  
  Received：15 January 2020，
  
  Revised：30 January 2020，
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Jun Xu, Nan-pu Cao, Yao-xin Xiao, Zhong-long Luo, Yu Bao, Shu-xun Cui. Revealing the Relationship between the Biocompatibility and the Bound Water of Poly(ethylene glycol) by Single-molecule Force Spectroscopy. [J]. Acta Polymerica Sinica 51(7):754-761(2020)
DOI：

Jun Xu, Nan-pu Cao, Yao-xin Xiao, Zhong-long Luo, Yu Bao, Shu-xun Cui. Revealing the Relationship between the Biocompatibility and the Bound Water of Poly(ethylene glycol) by Single-molecule Force Spectroscopy. [J]. Acta Polymerica Sinica 51(7):754-761(2020) DOI： 10.11777/j.issn1000-3304.2019.19219.

摘要

聚乙二醇(PEG)优良的生物相容性使得其在生物材料领域的应用十分广泛，但关于其具有良好生物相容性的分子机理依然不清楚. 本文利用单分子力谱技术研究了PEG生物相容性与其结合水之间的关系. PEG在非极性有机溶剂-壬烷及磷酸盐缓冲液(PBS)中的力-距离(

)曲线之间存在显著的差异. 通过实验分析及单分子理论模型验证发现这一差异主要是由PEG结合水重排所导致的. 对壬烷及PBS中的

曲线间的面积差进行积分得到PEG结合水重排所额外消耗的能量(

)为 ~ 1.59

/unit (3.93 kJ/mol). 通过对比发现，此

与生物大分子的

最为接近. 我们推测这一与生物大分子相近的

值保证了PEG在生物体内既不会引起严重的能量波动也不会影响其他分子的行为，这可能是PEG具有优良生物相容性的一个重要因素.

Abstract

Poly(ethylene glycol) (PEG) has become the “superstar” in the field of biological materials due to its excellent biocompatibility. However

the molecular mechanism underlying its biocompatibility is still unclear. In this work

we have investigated the relationship between the biocompatibility and the bound water of PEG by single-molecule force spectroscopy (SMFS). To discern the effect of bound water on PEG in an aqueous solution

the single-chain inherent elasticity of PEG should be determined first as a reference. The inherent elasticity of PEG is obtained in a small-sized nonpolar organic solvent

nonane

which is confirmed by the quantum mechanical calculations-based freely rotating chain model (QM-FRC model). Then

SMFS experiments have been performed in phosphate-buffered saline (PBS) to study the effect of bound water on PEG. The shoulder plateau in the force-extension (

) curve of PEG obtained in PBS should be caused by the rearrangement of the bound water (water bridge) during the PEG elongation. This assumption has been confirmed by the two states QM-FRC model (TSQM-FRC model)

which takes into account the effect of the water bridge. This bound water rearrangement will consume additional energy (

) besides that for the inherent elasticity of the chain. This

is calculated to be ~ 1.59

/unit (3.93 kJ/mol) by integrating the area between the

curves of PEG obtained in PBS and nonane

closed to those of biomacromolecules. Inspired by the relationship between the low

and the behaviors of biomacromolecules

we have speculated the relationship between the biocompatibility and the bound water of PEG: (1) Like those of biomacromolecules

this

makes sure that the conformational transition of PEG in blood or cell will not consume (or produce) too much energy. Thus

the energy disturbance caused by PEG can be borne by the organism. (2) An appropriate

can prevent the aggregation of biomacromolecules and PEG. Biomacromolecules can self-assemble into the high-level structure after partial dehydration. If PEG has no bound water (

= 0)

PEG may aggregate with the partially dehydrated biomacromolecules and then cause a series of consequences. In one word

the

closed to those of biomacromolecules may be an important factor for the excellent biocompatibility of PEG.

关键词

聚乙二醇生物相容性结合水单分子力谱

Keywords

Poly(ethylene glycol)BiocompatibilityBound waterSingle-molecule force spectroscopy

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College of Chemistry, Key Laboratory of Advanced Technologies of Materials (Ministry of Education), Southwest Jiaotong University

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering of China, Sichuan University

Key Lab of Advanced Technologies of Materials, Ministry of Education, Southwest Jiaotong University

Department of Pharmaceutical Engineering, School of Medical Engineering, Hefei University of Technology

Department of Chemical Technology, School of Environmental and Chemical Engineering, Yanshan University, Qinghuangdao

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