Bimetallic Single-Atom Nanozyme-Based Electrochemical-Photothermal Dual-Function Portable Immunoassay with Smartphone Imaging
Rapid and accurate detection of human epidermal growth factor receptor 2 (HER2) is crucial for the early diagnosis and prognosis of breast cancer. In this study, we reported an iron–manganese ion N-doped carbon single-atom catalyst (FeMn-NCetch/SAC) bimetallic peroxidase mimetic enzyme with abundant...
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| Veröffentlicht in: | Analytical chemistry (Washington) 2024-08, Vol.96 (33), p.13663-13671 |
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| creator | Wang, Yunsen Zeng, Ruijin Tian, Shuo Chen, Shuyun Bi, Zhilan Tang, Dianping Knopp, Dietmar |
| description | Rapid and accurate detection of human epidermal growth factor receptor 2 (HER2) is crucial for the early diagnosis and prognosis of breast cancer. In this study, we reported an iron–manganese ion N-doped carbon single-atom catalyst (FeMn-NCetch/SAC) bimetallic peroxidase mimetic enzyme with abundant active sites etched by H2O2 and further demonstrated unique advantages of single-atom bimetallic nanozymes in generating hydroxyl radicals by density functional theory (DFT) calculations. As a proof of concept, a portable device-dependent electrochemical-photothermal bifunctional immunoassay detection platform was designed to achieve reliable detection of HER2. In the enzyme-linked reaction, H2O2 was generated by substrate catalysis via secondary antibody-labeled glucose oxidase (GOx), while FeMn-NCetch/SAC nanozymes catalyzed the decomposition of H2O2 to form OH*, which catalyzed the conversion of 3,3′,5,5′-tetramethylbenzidine (TMB) to ox-TMB. The ox-TMB generation was converted from the colorimetric signals to electrical and photothermal signals by applied potential and laser irradiation, which could be employed for the quantitative detection of HER2. With the help of this bifunctional detection technology, HER2 was accurately detected in two ways: photothermally, with a linear scope of 0.01 to 2.0 ng mL–1 and a limit of detection (LOD) of 7.5 pg mL–1, and electrochemically, with a linear scope of 0.01 to 10 ng mL–1 at an LOD of 3.9 pg mL–1. By successfully avoiding environmental impacts, the bifunctional-based immunosensing strategy offers strong support for accurate clinical detection. |
| doi_str_mv | 10.1021/acs.analchem.4c02606 |
| format | Article |
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In this study, we reported an iron–manganese ion N-doped carbon single-atom catalyst (FeMn-NCetch/SAC) bimetallic peroxidase mimetic enzyme with abundant active sites etched by H2O2 and further demonstrated unique advantages of single-atom bimetallic nanozymes in generating hydroxyl radicals by density functional theory (DFT) calculations. As a proof of concept, a portable device-dependent electrochemical-photothermal bifunctional immunoassay detection platform was designed to achieve reliable detection of HER2. In the enzyme-linked reaction, H2O2 was generated by substrate catalysis via secondary antibody-labeled glucose oxidase (GOx), while FeMn-NCetch/SAC nanozymes catalyzed the decomposition of H2O2 to form OH*, which catalyzed the conversion of 3,3′,5,5′-tetramethylbenzidine (TMB) to ox-TMB. The ox-TMB generation was converted from the colorimetric signals to electrical and photothermal signals by applied potential and laser irradiation, which could be employed for the quantitative detection of HER2. With the help of this bifunctional detection technology, HER2 was accurately detected in two ways: photothermally, with a linear scope of 0.01 to 2.0 ng mL–1 and a limit of detection (LOD) of 7.5 pg mL–1, and electrochemically, with a linear scope of 0.01 to 10 ng mL–1 at an LOD of 3.9 pg mL–1. By successfully avoiding environmental impacts, the bifunctional-based immunosensing strategy offers strong support for accurate clinical detection.</description><identifier>ISSN: 0003-2700</identifier><identifier>ISSN: 1520-6882</identifier><identifier>EISSN: 1520-6882</identifier><identifier>DOI: 10.1021/acs.analchem.4c02606</identifier><identifier>PMID: 39126679</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Benzidines - chemistry ; Bimetals ; Breast Neoplasms ; Catalysis ; Catalysts ; Colorimetry ; Decomposition reactions ; Density Functional Theory ; Electrochemical Techniques ; Electrochemistry ; Environmental impact ; Enzymes ; ErbB-2 protein ; Free radicals ; Glucose oxidase ; Glucose Oxidase - chemistry ; Glucose Oxidase - metabolism ; Growth factors ; Humans ; Hydrogen peroxide ; Hydrogen Peroxide - analysis ; Hydrogen Peroxide - chemistry ; Hydroxyl radicals ; Immunoassay ; Immunoassay - methods ; Immunosensors ; Iron - chemistry ; Irradiation ; Laser radiation ; Limit of Detection ; Manganese ; Manganese - chemistry ; Manganese ions ; Peroxidase ; Photothermal conversion ; Portable equipment ; Receptor, ErbB-2 - analysis ; Receptor, ErbB-2 - immunology ; Signal generation ; Single atom catalysts ; Smartphone ; Substrates</subject><ispartof>Analytical chemistry (Washington), 2024-08, Vol.96 (33), p.13663-13671</ispartof><rights>2024 The Authors. Published by American Chemical Society</rights><rights>Copyright American Chemical Society Aug 20, 2024</rights><rights>2024 The Authors. Published by American Chemical Society 2024 The Authors</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-a311t-b2c98279db180ef57db1af51dc3127fc809d26bbabdd81312f38b1a191e17d353</cites><orcidid>0000-0003-4566-9798 ; 0000-0002-0134-3983</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.analchem.4c02606$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.analchem.4c02606$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,780,784,885,2763,27074,27922,27923,56736,56786</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/39126679$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Wang, Yunsen</creatorcontrib><creatorcontrib>Zeng, Ruijin</creatorcontrib><creatorcontrib>Tian, Shuo</creatorcontrib><creatorcontrib>Chen, Shuyun</creatorcontrib><creatorcontrib>Bi, Zhilan</creatorcontrib><creatorcontrib>Tang, Dianping</creatorcontrib><creatorcontrib>Knopp, Dietmar</creatorcontrib><title>Bimetallic Single-Atom Nanozyme-Based Electrochemical-Photothermal Dual-Function Portable Immunoassay with Smartphone Imaging</title><title>Analytical chemistry (Washington)</title><addtitle>Anal. Chem</addtitle><description>Rapid and accurate detection of human epidermal growth factor receptor 2 (HER2) is crucial for the early diagnosis and prognosis of breast cancer. In this study, we reported an iron–manganese ion N-doped carbon single-atom catalyst (FeMn-NCetch/SAC) bimetallic peroxidase mimetic enzyme with abundant active sites etched by H2O2 and further demonstrated unique advantages of single-atom bimetallic nanozymes in generating hydroxyl radicals by density functional theory (DFT) calculations. As a proof of concept, a portable device-dependent electrochemical-photothermal bifunctional immunoassay detection platform was designed to achieve reliable detection of HER2. In the enzyme-linked reaction, H2O2 was generated by substrate catalysis via secondary antibody-labeled glucose oxidase (GOx), while FeMn-NCetch/SAC nanozymes catalyzed the decomposition of H2O2 to form OH*, which catalyzed the conversion of 3,3′,5,5′-tetramethylbenzidine (TMB) to ox-TMB. The ox-TMB generation was converted from the colorimetric signals to electrical and photothermal signals by applied potential and laser irradiation, which could be employed for the quantitative detection of HER2. With the help of this bifunctional detection technology, HER2 was accurately detected in two ways: photothermally, with a linear scope of 0.01 to 2.0 ng mL–1 and a limit of detection (LOD) of 7.5 pg mL–1, and electrochemically, with a linear scope of 0.01 to 10 ng mL–1 at an LOD of 3.9 pg mL–1. By successfully avoiding environmental impacts, the bifunctional-based immunosensing strategy offers strong support for accurate clinical detection.</description><subject>Benzidines - chemistry</subject><subject>Bimetals</subject><subject>Breast Neoplasms</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Colorimetry</subject><subject>Decomposition reactions</subject><subject>Density Functional Theory</subject><subject>Electrochemical Techniques</subject><subject>Electrochemistry</subject><subject>Environmental impact</subject><subject>Enzymes</subject><subject>ErbB-2 protein</subject><subject>Free radicals</subject><subject>Glucose oxidase</subject><subject>Glucose Oxidase - chemistry</subject><subject>Glucose Oxidase - metabolism</subject><subject>Growth factors</subject><subject>Humans</subject><subject>Hydrogen peroxide</subject><subject>Hydrogen Peroxide - analysis</subject><subject>Hydrogen Peroxide - chemistry</subject><subject>Hydroxyl radicals</subject><subject>Immunoassay</subject><subject>Immunoassay - methods</subject><subject>Immunosensors</subject><subject>Iron - chemistry</subject><subject>Irradiation</subject><subject>Laser radiation</subject><subject>Limit of Detection</subject><subject>Manganese</subject><subject>Manganese - chemistry</subject><subject>Manganese ions</subject><subject>Peroxidase</subject><subject>Photothermal conversion</subject><subject>Portable equipment</subject><subject>Receptor, ErbB-2 - analysis</subject><subject>Receptor, ErbB-2 - immunology</subject><subject>Signal generation</subject><subject>Single atom catalysts</subject><subject>Smartphone</subject><subject>Substrates</subject><issn>0003-2700</issn><issn>1520-6882</issn><issn>1520-6882</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNp9kU9v1DAQxSMEokvhGyAUiUsvWTz2buKcUFvaUqmCSoWzNXGcjSv_WWwHtEh893rZ7Qo4cLI185v3xn5F8RrIHAiFdyjjHB0aOSo7X0hCa1I_KWawpKSqOadPixkhhFW0IeSoeBHjPSEABOrnxRFrgdZ1086KX2faqoTGaFneabcyqjpN3paf0PmfG6uqM4yqLy-Mkin4rZeWaKrb0SefRhUsmvLDlCuXk5NJe1fe-pCwM6q8tnZyHmPETflDp7G8sxjSevRu28NVdntZPBvQRPVqfx4XXy8vvpx_rG4-X12fn95UyABS1VHZctq0fQecqGHZ5AsOS-glA9oMkpO2p3XXYdf3HHJtYDwT0IKCpmdLdly83-mup86qXiqXAhqxDjqvtBEetfi74_QoVv67AGCsbegiK5zsFYL_NqmYhNVRKmPQKT9FwUj-Ut7wps3o23_Qez-FnNRvijMCtIVMLXaUDD7GoIbDNkDENmCRAxaPAYt9wHnszZ8vOQw9JpoBsgO24wfj_2o-ALQVuGI</recordid><startdate>20240820</startdate><enddate>20240820</enddate><creator>Wang, Yunsen</creator><creator>Zeng, Ruijin</creator><creator>Tian, Shuo</creator><creator>Chen, Shuyun</creator><creator>Bi, Zhilan</creator><creator>Tang, Dianping</creator><creator>Knopp, Dietmar</creator><general>American Chemical Society</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QF</scope><scope>7QO</scope><scope>7QQ</scope><scope>7SC</scope><scope>7SE</scope><scope>7SP</scope><scope>7SR</scope><scope>7TA</scope><scope>7TB</scope><scope>7TM</scope><scope>7U5</scope><scope>7U7</scope><scope>7U9</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>H8G</scope><scope>H94</scope><scope>JG9</scope><scope>JQ2</scope><scope>KR7</scope><scope>L7M</scope><scope>L~C</scope><scope>L~D</scope><scope>P64</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0003-4566-9798</orcidid><orcidid>https://orcid.org/0000-0002-0134-3983</orcidid></search><sort><creationdate>20240820</creationdate><title>Bimetallic Single-Atom Nanozyme-Based Electrochemical-Photothermal Dual-Function Portable Immunoassay with Smartphone Imaging</title><author>Wang, Yunsen ; 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Chem</addtitle><date>2024-08-20</date><risdate>2024</risdate><volume>96</volume><issue>33</issue><spage>13663</spage><epage>13671</epage><pages>13663-13671</pages><issn>0003-2700</issn><issn>1520-6882</issn><eissn>1520-6882</eissn><abstract>Rapid and accurate detection of human epidermal growth factor receptor 2 (HER2) is crucial for the early diagnosis and prognosis of breast cancer. In this study, we reported an iron–manganese ion N-doped carbon single-atom catalyst (FeMn-NCetch/SAC) bimetallic peroxidase mimetic enzyme with abundant active sites etched by H2O2 and further demonstrated unique advantages of single-atom bimetallic nanozymes in generating hydroxyl radicals by density functional theory (DFT) calculations. As a proof of concept, a portable device-dependent electrochemical-photothermal bifunctional immunoassay detection platform was designed to achieve reliable detection of HER2. In the enzyme-linked reaction, H2O2 was generated by substrate catalysis via secondary antibody-labeled glucose oxidase (GOx), while FeMn-NCetch/SAC nanozymes catalyzed the decomposition of H2O2 to form OH*, which catalyzed the conversion of 3,3′,5,5′-tetramethylbenzidine (TMB) to ox-TMB. The ox-TMB generation was converted from the colorimetric signals to electrical and photothermal signals by applied potential and laser irradiation, which could be employed for the quantitative detection of HER2. With the help of this bifunctional detection technology, HER2 was accurately detected in two ways: photothermally, with a linear scope of 0.01 to 2.0 ng mL–1 and a limit of detection (LOD) of 7.5 pg mL–1, and electrochemically, with a linear scope of 0.01 to 10 ng mL–1 at an LOD of 3.9 pg mL–1. By successfully avoiding environmental impacts, the bifunctional-based immunosensing strategy offers strong support for accurate clinical detection.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>39126679</pmid><doi>10.1021/acs.analchem.4c02606</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0003-4566-9798</orcidid><orcidid>https://orcid.org/0000-0002-0134-3983</orcidid><oa>free_for_read</oa></addata></record> |
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| subjects | Benzidines - chemistry Bimetals Breast Neoplasms Catalysis Catalysts Colorimetry Decomposition reactions Density Functional Theory Electrochemical Techniques Electrochemistry Environmental impact Enzymes ErbB-2 protein Free radicals Glucose oxidase Glucose Oxidase - chemistry Glucose Oxidase - metabolism Growth factors Humans Hydrogen peroxide Hydrogen Peroxide - analysis Hydrogen Peroxide - chemistry Hydroxyl radicals Immunoassay Immunoassay - methods Immunosensors Iron - chemistry Irradiation Laser radiation Limit of Detection Manganese Manganese - chemistry Manganese ions Peroxidase Photothermal conversion Portable equipment Receptor, ErbB-2 - analysis Receptor, ErbB-2 - immunology Signal generation Single atom catalysts Smartphone Substrates |
| title | Bimetallic Single-Atom Nanozyme-Based Electrochemical-Photothermal Dual-Function Portable Immunoassay with Smartphone Imaging |
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