{"title":"基于In2S3和Cu2ZnSnS4之间硼酯桥接的极性可切换光电化学检测酪氨酸酶活性。","authors":"Rong Liao, Bowen Yan, Shihua Wang, Wenfang Deng, Yueming Tan, Qingji Xie","doi":"10.1016/j.talanta.2025.128405","DOIUrl":null,"url":null,"abstract":"<p><p>Herein, an innovative polarity switchable strategy for photoelectrochemical (PEC) detection is reported by utilizing enzyme-triggered boronic ester bridging between two semiconductors. Monophenol-modified In<sub>2</sub>S<sub>3</sub> is prepared by sequentially coating polyethyleneimine (PEI) and covalently conjugating 4-hydroxyphenylacetic acid (PhOH) on In<sub>2</sub>S<sub>3</sub>, whereas dihydroxy-modified Cu<sub>2</sub>ZnSnS<sub>4</sub> is prepared through surface coating of chitosan (CS). Under the catalysis of tyrosinase (TYR), monophenol groups of In<sub>2</sub>S<sub>3</sub>@PEI-PhOH undergo the conversion to o-diphenol groups. With the aid of 1,4-phenylboronic acid, boronate ester bridges form between TYR-treated In<sub>2</sub>S<sub>3</sub>@PEI-PhOH and Cu<sub>2</sub>ZnSnS<sub>4</sub>@CS, so In<sub>2</sub>S<sub>3</sub> can be anchored on the Cu<sub>2</sub>ZnSnS<sub>4</sub>@CS-modified electrode surface. As a result, the formation of p-n heterojunctions on the photoelectrode can reverse the photocurrent polarity, enabling polarity switchable PEC detection of TYR activity. The linear range is from 0.01 to 5 U mL<sup>-1</sup>, and the detection limit is 0.0015 U mL<sup>-1</sup> for TYR activity detection. The established method is successfully employed for TYR activity detection in human serum samples.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"295 ","pages":"128405"},"PeriodicalIF":6.1000,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Polarity-switchable photoelectrochemical detection of tyrosinase activity based on enzyme-triggered boronic ester bridging between In<sub>2</sub>S<sub>3</sub> and Cu<sub>2</sub>ZnSnS<sub>4</sub>.\",\"authors\":\"Rong Liao, Bowen Yan, Shihua Wang, Wenfang Deng, Yueming Tan, Qingji Xie\",\"doi\":\"10.1016/j.talanta.2025.128405\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Herein, an innovative polarity switchable strategy for photoelectrochemical (PEC) detection is reported by utilizing enzyme-triggered boronic ester bridging between two semiconductors. Monophenol-modified In<sub>2</sub>S<sub>3</sub> is prepared by sequentially coating polyethyleneimine (PEI) and covalently conjugating 4-hydroxyphenylacetic acid (PhOH) on In<sub>2</sub>S<sub>3</sub>, whereas dihydroxy-modified Cu<sub>2</sub>ZnSnS<sub>4</sub> is prepared through surface coating of chitosan (CS). Under the catalysis of tyrosinase (TYR), monophenol groups of In<sub>2</sub>S<sub>3</sub>@PEI-PhOH undergo the conversion to o-diphenol groups. With the aid of 1,4-phenylboronic acid, boronate ester bridges form between TYR-treated In<sub>2</sub>S<sub>3</sub>@PEI-PhOH and Cu<sub>2</sub>ZnSnS<sub>4</sub>@CS, so In<sub>2</sub>S<sub>3</sub> can be anchored on the Cu<sub>2</sub>ZnSnS<sub>4</sub>@CS-modified electrode surface. As a result, the formation of p-n heterojunctions on the photoelectrode can reverse the photocurrent polarity, enabling polarity switchable PEC detection of TYR activity. The linear range is from 0.01 to 5 U mL<sup>-1</sup>, and the detection limit is 0.0015 U mL<sup>-1</sup> for TYR activity detection. The established method is successfully employed for TYR activity detection in human serum samples.</p>\",\"PeriodicalId\":435,\"journal\":{\"name\":\"Talanta\",\"volume\":\"295 \",\"pages\":\"128405\"},\"PeriodicalIF\":6.1000,\"publicationDate\":\"2025-12-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Talanta\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.talanta.2025.128405\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/5/27 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Talanta","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.talanta.2025.128405","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/5/27 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0
摘要
本文报道了一种利用酶触发的硼酯桥接在两个半导体之间进行光电化学（PEC）检测的创新极性切换策略。采用聚亚胺（PEI）和4-羟基苯基乙酸（PhOH）在In2S3表面依次包覆制备了单酚改性In2S3，采用壳聚糖（CS）表面包覆制备了二羟基改性Cu2ZnSnS4。在酪氨酸酶（TYR）的催化下，In2S3@PEI-PhOH的单酚基团转化为邻二酚基团。在1,4-苯硼酸的帮助下，硼酸酯桥接在tyrr处理过的In2S3@PEI-PhOH和Cu2ZnSnS4@CS之间，因此In2S3可以锚定在Cu2ZnSnS4@CS-modified电极表面。因此，在光电极上形成p-n异质结可以逆转光电流极性，使极性可切换的PEC检测TYR活性成为可能。线性范围为0.01 ~ 5 U mL-1，检出限为0.0015 U mL-1。建立的方法成功地用于人血清样品中TYR活性的检测。
Polarity-switchable photoelectrochemical detection of tyrosinase activity based on enzyme-triggered boronic ester bridging between In2S3 and Cu2ZnSnS4.
Herein, an innovative polarity switchable strategy for photoelectrochemical (PEC) detection is reported by utilizing enzyme-triggered boronic ester bridging between two semiconductors. Monophenol-modified In2S3 is prepared by sequentially coating polyethyleneimine (PEI) and covalently conjugating 4-hydroxyphenylacetic acid (PhOH) on In2S3, whereas dihydroxy-modified Cu2ZnSnS4 is prepared through surface coating of chitosan (CS). Under the catalysis of tyrosinase (TYR), monophenol groups of In2S3@PEI-PhOH undergo the conversion to o-diphenol groups. With the aid of 1,4-phenylboronic acid, boronate ester bridges form between TYR-treated In2S3@PEI-PhOH and Cu2ZnSnS4@CS, so In2S3 can be anchored on the Cu2ZnSnS4@CS-modified electrode surface. As a result, the formation of p-n heterojunctions on the photoelectrode can reverse the photocurrent polarity, enabling polarity switchable PEC detection of TYR activity. The linear range is from 0.01 to 5 U mL-1, and the detection limit is 0.0015 U mL-1 for TYR activity detection. The established method is successfully employed for TYR activity detection in human serum samples.
期刊介绍：
Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome.
Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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