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Biomimetic nanochannels for the discrimination of sialylated glycans via a tug-of-war between glycan binding and polymer shrinkage

发表时间:2020-02-17
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论文类型:
期刊论文
第一作者:
Li, Minmin
通讯作者:
Liang, XM; Qing, GY (reprint author), Chinese Acad Sci, Dalian Inst Chem Phys, Key Lab Separat Sci Analyt Chem, 457 Zhongshan Rd, Dalian 116023, Peoples R China.
合写作者:
Xiong, Yuting,Wang, Dongdong,Liu, Yunhai,Na, Bing,Qin, Haijuan,Liu, Jinxuan,Liang, Xinmiao,Qing, Guangyan
发表时间:
2020-01-21
发表刊物:
CHEMICAL SCIENCE
收录刊物:
EI、SCIE
文献类型:
J
卷号:
11
期号:
3
页面范围:
748-756
ISSN号:
2041-6520
摘要:
Sialylated glycans that are attached to cell surface mediate diverse cellular processes such as immune responses, pathogen binding, and cancer progression. Precise determination of sialylated glycans, particularly their linkage isomers that can trigger distinct biological events and are indicative of different cancer types, remains a challenge, due to their complicated composition and limited structural differences. Here, we present a biomimetic nanochannels system integrated with the responsive polymer polyethyleneimine-g-glucopyranoside (Glc-PEI) to solve this problem. By using a dramatic "OFF-ON" change in ion flux, the nanochannels system achieves specific recognition for N-acetylneuraminic acid (Neu5Ac, the predominant form of sialic acid) from various monosaccharides and sialic acid species. Importantly, different "OFF-ON" ratios of the conical nanochannels system allows the precise and sensitive discrimination of sialylated glycan linkage isomers, alpha 2-3 and alpha 2-6 linkage (the corresponding ion conductance increase ratios are 96.2% and 264%, respectively). Analyses revealed an unusual tug-of-war mechanism between polymer-glycan binding and polymer shrinkage. The low binding affinity of Glc-PEI for the alpha 2-6-linked glycan caused considerable shrinkage of Glc-PEI layer, but the high affinity for the alpha 2-3-linked glycan resulted in only a slight shrinkage. This competition mechanism provides a simple and versatile materials design principle for recognition or sensing systems that involve negatively charged target biomolecules. Furthermore, this work broadens the application of nanochannel systems in bioanalysis and biosensing, and opens a new route to glycan analysis that could help to uncover the mysterious and wonderful glycoworld.
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