Mubalake Rehemaitijiang, Gaosheng Li, Rongchao Zhu, Baiyi Zu, Xincun Dou, Zhi Su, Zhenzhen Cai
{"title":"精确斯托克斯移位调制在D-π-A化学剂量计中实现三标准次氯酸盐定量阵列","authors":"Mubalake Rehemaitijiang, Gaosheng Li, Rongchao Zhu, Baiyi Zu, Xincun Dou, Zhi Su, Zhenzhen Cai","doi":"10.1021/acs.analchem.5c00821","DOIUrl":null,"url":null,"abstract":"The rational design of the D-π-A chemodosimeter with a significant Stokes shift is of great importance for enhancing the visualization of optical sensing signals. Here, three D-π-A fluorescent chemodosimeters with 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene) malononitrile (TCF) as the electron-withdrawing group are synthesized by precisely modulating the electron-releasing strength. By decreasing the ability of electron release, the electrophilicity of the recognition site is increased by 1.449 kcal/mol, the Stokes shift of the chemodosimeter is improved to 201 nm, and the sensing mode changes from fluorescence quenching to ratiometric fluorescence and finally to fluorescence on. Furthermore, the three D-π-A fluorescent chemodosimeters display superior sensing performance toward ClO<sup>–</sup>, including low limits of detection (LOD, 37.0, 5.1, and 1.0 nM), rapid response (<5 s), and great selectivity in the presence of 16 kinds of interferents. Moreover, the practicality of the chemodosimeters is further validated by a portable triple-standard quantitative array detection platform, which can quantitatively detect ClO<sup>–</sup> solutions. The proposed design and modulation strategy for chemodosimeters can provide a new pathway for the sensitive and visualized identification of oxidants and other hazardous chemicals.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"2 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Triple-Standard Hypochlorite Quantitative Array Enabled by Precise Stokes Shift Modulation in D-π-A Chemodosimeters\",\"authors\":\"Mubalake Rehemaitijiang, Gaosheng Li, Rongchao Zhu, Baiyi Zu, Xincun Dou, Zhi Su, Zhenzhen Cai\",\"doi\":\"10.1021/acs.analchem.5c00821\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The rational design of the D-π-A chemodosimeter with a significant Stokes shift is of great importance for enhancing the visualization of optical sensing signals. Here, three D-π-A fluorescent chemodosimeters with 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene) malononitrile (TCF) as the electron-withdrawing group are synthesized by precisely modulating the electron-releasing strength. By decreasing the ability of electron release, the electrophilicity of the recognition site is increased by 1.449 kcal/mol, the Stokes shift of the chemodosimeter is improved to 201 nm, and the sensing mode changes from fluorescence quenching to ratiometric fluorescence and finally to fluorescence on. Furthermore, the three D-π-A fluorescent chemodosimeters display superior sensing performance toward ClO<sup>–</sup>, including low limits of detection (LOD, 37.0, 5.1, and 1.0 nM), rapid response (<5 s), and great selectivity in the presence of 16 kinds of interferents. Moreover, the practicality of the chemodosimeters is further validated by a portable triple-standard quantitative array detection platform, which can quantitatively detect ClO<sup>–</sup> solutions. The proposed design and modulation strategy for chemodosimeters can provide a new pathway for the sensitive and visualized identification of oxidants and other hazardous chemicals.\",\"PeriodicalId\":27,\"journal\":{\"name\":\"Analytical Chemistry\",\"volume\":\"2 1\",\"pages\":\"\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2025-04-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Analytical Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.analchem.5c00821\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.analchem.5c00821","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Triple-Standard Hypochlorite Quantitative Array Enabled by Precise Stokes Shift Modulation in D-π-A Chemodosimeters
The rational design of the D-π-A chemodosimeter with a significant Stokes shift is of great importance for enhancing the visualization of optical sensing signals. Here, three D-π-A fluorescent chemodosimeters with 2-(3-cyano-4,5,5-trimethylfuran-2(5H)-ylidene) malononitrile (TCF) as the electron-withdrawing group are synthesized by precisely modulating the electron-releasing strength. By decreasing the ability of electron release, the electrophilicity of the recognition site is increased by 1.449 kcal/mol, the Stokes shift of the chemodosimeter is improved to 201 nm, and the sensing mode changes from fluorescence quenching to ratiometric fluorescence and finally to fluorescence on. Furthermore, the three D-π-A fluorescent chemodosimeters display superior sensing performance toward ClO–, including low limits of detection (LOD, 37.0, 5.1, and 1.0 nM), rapid response (<5 s), and great selectivity in the presence of 16 kinds of interferents. Moreover, the practicality of the chemodosimeters is further validated by a portable triple-standard quantitative array detection platform, which can quantitatively detect ClO– solutions. The proposed design and modulation strategy for chemodosimeters can provide a new pathway for the sensitive and visualized identification of oxidants and other hazardous chemicals.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.