{"title":"Engineering Bio-Inspired Nanochannels with pH-Responsive Gates for Direct Detection of Glucose in Human Blood Serum","authors":"Yinde Wu, Jialun Li, Yunzhou Chen, Xuancheng Liu, Yueyang Zhang, Chongxuan Xiao, Zihao Li, Yan-Yan Song, Tian Shen, Xiaona Li","doi":"10.1016/j.aca.2025.343973","DOIUrl":null,"url":null,"abstract":"<h3>Background</h3>An abnormal blood glucose (Glu) level is a key signal of diabetes. The gluconic acid produced by Glu catalytic oxidation can cause changes in pH value.<h3>Results</h3>Inspired by nature, in which organisms use pH as a chemical gate to regulate ion transport through cell membranes, we report a pH-gated electrochemical luminescence (ECL) sensing system for Glu detection based on the relationship between Glu metabolism and pH. The pH gate was designed on a TiO<sub>2</sub> nanochannel membrane (NM) by modifying the channel entrance with polystyrene-b-poly(4-vinylpyridine) (P4VP) chains that convert from a hydrophobic into a hydrophilic state via a pH-responsive conformational switching at pKa 5.2. Due to the nanoconfinement effect of zeolite imidazolate (ZIF-8) frameworks and TiO<sub>2</sub> nanochannels, the glucose oxidase (GOD) embedded in ZIF-8 exhibits enhanced catalytic efficiency for Glu oxidation, enabling the acidic product to regulate the hydrophilicity of the P4VP-based pH-responsive gate. The ECL luminophore Ru(dcbpy)<sub>3</sub><sup>2+</sup> subsequently passes through the hydrophilic gate to reach the detection cell. This pH-gated Glu-responsive NM can effectively separate biological matrices from the detection cell, allowing direct sensing of Glu in complex biomatrices.<h3>Significance</h3>The ECL technology, combined with the pH-triggered gate design enables straightforward Glu determination in undiluted serum, demonstrating an alternative ECL device for pretreatment-free clinical analysis.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"11 1","pages":""},"PeriodicalIF":5.7000,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.aca.2025.343973","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Background
An abnormal blood glucose (Glu) level is a key signal of diabetes. The gluconic acid produced by Glu catalytic oxidation can cause changes in pH value.
Results
Inspired by nature, in which organisms use pH as a chemical gate to regulate ion transport through cell membranes, we report a pH-gated electrochemical luminescence (ECL) sensing system for Glu detection based on the relationship between Glu metabolism and pH. The pH gate was designed on a TiO2 nanochannel membrane (NM) by modifying the channel entrance with polystyrene-b-poly(4-vinylpyridine) (P4VP) chains that convert from a hydrophobic into a hydrophilic state via a pH-responsive conformational switching at pKa 5.2. Due to the nanoconfinement effect of zeolite imidazolate (ZIF-8) frameworks and TiO2 nanochannels, the glucose oxidase (GOD) embedded in ZIF-8 exhibits enhanced catalytic efficiency for Glu oxidation, enabling the acidic product to regulate the hydrophilicity of the P4VP-based pH-responsive gate. The ECL luminophore Ru(dcbpy)32+ subsequently passes through the hydrophilic gate to reach the detection cell. This pH-gated Glu-responsive NM can effectively separate biological matrices from the detection cell, allowing direct sensing of Glu in complex biomatrices.
Significance
The ECL technology, combined with the pH-triggered gate design enables straightforward Glu determination in undiluted serum, demonstrating an alternative ECL device for pretreatment-free clinical analysis.
期刊介绍:
Analytica Chimica Acta has an open access mirror journal Analytica Chimica Acta: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review.
Analytica Chimica Acta provides a forum for the rapid publication of original research, and critical, comprehensive reviews dealing with all aspects of fundamental and applied modern analytical chemistry. The journal welcomes the submission of research papers which report studies concerning the development of new and significant analytical methodologies. In determining the suitability of submitted articles for publication, particular scrutiny will be placed on the degree of novelty and impact of the research and the extent to which it adds to the existing body of knowledge in analytical chemistry.