{"title":"具有接近效应和对底物极性增强的硅酸锰用于高效酶促生物传感","authors":"Jianyu Huang, Xiaowei Li*, Xiuling Li, Longjie Zhang, Yingqian Chu, Enxiang Jiao*, Guangwu Wen and Zhihui Niu*, ","doi":"10.1021/acsami.4c2264510.1021/acsami.4c22645","DOIUrl":null,"url":null,"abstract":"<p >Functional nanoparticle-mediated enzymatic sensors have been extensively utilized in the colorimetric detection of biomolecules. However, low affinity toward substrates and unstable color development of oxidized substrates severely influence the detection period and reliability of results. Herein, a rapid and reliable method has been proposed by employing manganese silicate NPs (MSs) as the paradigm for enzymatic colorimetric detection of uric acid (UA). MSs demonstrate favorable catalytic kinetics (<i>K</i><sub>m</sub> = 0.046 mM). Compared with reported methods, the shortened detection period and ultralong enzymatic curve platform (∼8 min) ensure higher rapidity and reliability. Theoretical calculations based on density functional theory were further utilized to reveal the catalytic mechanism of the MSs oxidase mimic. The inherent ability to spontaneously generate ROS along with its proximity effect resulting from substrate adsorption provides robust theoretical support for ultrafast catalytic kinetics. Moreover, silicate ions reduced the degree of electron delocalization in oxidized TMB with increasing molecular polarity and decreased the solvation free energy to further improve the dissolution stability. As expected, the MSs-based method exhibits excellent accuracy and higher stability in monitoring UA change of human urine specimens, which is superior to the commercial kit. Furthermore, the integration of colorimetric methodologies with portable smart detection systems bridges fundamental scientific exploration and practical implementation, enabling both a reduced detection cost and expanded applicability of nanozyme-based sensors.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"17 18","pages":"26191–26201 26191–26201"},"PeriodicalIF":8.2000,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Manganese Silicate with Proximity Effect and Enhanced Polarity toward Substrates for Efficient Enzymatic Biosensing\",\"authors\":\"Jianyu Huang, Xiaowei Li*, Xiuling Li, Longjie Zhang, Yingqian Chu, Enxiang Jiao*, Guangwu Wen and Zhihui Niu*, \",\"doi\":\"10.1021/acsami.4c2264510.1021/acsami.4c22645\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Functional nanoparticle-mediated enzymatic sensors have been extensively utilized in the colorimetric detection of biomolecules. However, low affinity toward substrates and unstable color development of oxidized substrates severely influence the detection period and reliability of results. Herein, a rapid and reliable method has been proposed by employing manganese silicate NPs (MSs) as the paradigm for enzymatic colorimetric detection of uric acid (UA). MSs demonstrate favorable catalytic kinetics (<i>K</i><sub>m</sub> = 0.046 mM). Compared with reported methods, the shortened detection period and ultralong enzymatic curve platform (∼8 min) ensure higher rapidity and reliability. Theoretical calculations based on density functional theory were further utilized to reveal the catalytic mechanism of the MSs oxidase mimic. The inherent ability to spontaneously generate ROS along with its proximity effect resulting from substrate adsorption provides robust theoretical support for ultrafast catalytic kinetics. Moreover, silicate ions reduced the degree of electron delocalization in oxidized TMB with increasing molecular polarity and decreased the solvation free energy to further improve the dissolution stability. As expected, the MSs-based method exhibits excellent accuracy and higher stability in monitoring UA change of human urine specimens, which is superior to the commercial kit. Furthermore, the integration of colorimetric methodologies with portable smart detection systems bridges fundamental scientific exploration and practical implementation, enabling both a reduced detection cost and expanded applicability of nanozyme-based sensors.</p>\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"17 18\",\"pages\":\"26191–26201 26191–26201\"},\"PeriodicalIF\":8.2000,\"publicationDate\":\"2025-04-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsami.4c22645\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsami.4c22645","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Manganese Silicate with Proximity Effect and Enhanced Polarity toward Substrates for Efficient Enzymatic Biosensing
Functional nanoparticle-mediated enzymatic sensors have been extensively utilized in the colorimetric detection of biomolecules. However, low affinity toward substrates and unstable color development of oxidized substrates severely influence the detection period and reliability of results. Herein, a rapid and reliable method has been proposed by employing manganese silicate NPs (MSs) as the paradigm for enzymatic colorimetric detection of uric acid (UA). MSs demonstrate favorable catalytic kinetics (Km = 0.046 mM). Compared with reported methods, the shortened detection period and ultralong enzymatic curve platform (∼8 min) ensure higher rapidity and reliability. Theoretical calculations based on density functional theory were further utilized to reveal the catalytic mechanism of the MSs oxidase mimic. The inherent ability to spontaneously generate ROS along with its proximity effect resulting from substrate adsorption provides robust theoretical support for ultrafast catalytic kinetics. Moreover, silicate ions reduced the degree of electron delocalization in oxidized TMB with increasing molecular polarity and decreased the solvation free energy to further improve the dissolution stability. As expected, the MSs-based method exhibits excellent accuracy and higher stability in monitoring UA change of human urine specimens, which is superior to the commercial kit. Furthermore, the integration of colorimetric methodologies with portable smart detection systems bridges fundamental scientific exploration and practical implementation, enabling both a reduced detection cost and expanded applicability of nanozyme-based sensors.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.