Enhanced Peroxidase-Mimic Catalytic Activity via Cerium Doping of Strontium-Based Metal–Organic Frameworks with Design of a Smartphone-Based Sensor for On-Site Salivary Total Antioxidant Capacity Detection in Lung Cancer Patients
The development of artificial nanozymes with superior catalytic performance and excellent stability has been a long-standing objective for chemists. The total antioxidant capacity (TAC) is one of the most important bioanalytical measures of oxidative stress in the body. The present work aims to deve...
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Veröffentlicht in: | ACS applied materials & interfaces 2023-05, Vol.15 (17), p.21239-21251 |
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description | The development of artificial nanozymes with superior catalytic performance and excellent stability has been a long-standing objective for chemists. The total antioxidant capacity (TAC) is one of the most important bioanalytical measures of oxidative stress in the body. The present work aims to develop a smartphone-assisted visual detection sensor using cerium-doped strontium-based metal–organic frameworks (Ce-SrMOFs) as peroxidase-like nanozymes for the rapid, low-cost, on-site detection of TAC. The pristine SrMOF functioned as a peroxidase nanozyme, and its enzymatic activity was enhanced after doping it with Ce(IV) ions because of the multivalent nature and synergistic impact of the heteroatoms. The Ce-SrMOFs were sensitive to the single electron transfer and hydrogen atom transfer processes, which implies that the Ce-SrMOFs can serve as an ideal nanozyme candidate for TAC analysis. The investigated mechanism revealed that •OH is the most active oxygen species for the peroxidase-like activity. The Ce-SrMOFs exhibited a strong affinity for 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2, with K m values of 0.082 and 0.427 mM, which are 5.29- and 8.67-fold lower than those of horseradish peroxidase (HRP), respectively. The Ce-SrMOFs were used for the detection of ascorbic acid, cysteine, and glutathione, with limits of detection of 44, 53, and 512 nM, respectively. The proposed method proved effective in measuring the TAC in saliva samples from lung cancer patients, thereby yielding results with satisfactory precision and accuracy. |
doi_str_mv | 10.1021/acsami.3c01007 |
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The total antioxidant capacity (TAC) is one of the most important bioanalytical measures of oxidative stress in the body. The present work aims to develop a smartphone-assisted visual detection sensor using cerium-doped strontium-based metal–organic frameworks (Ce-SrMOFs) as peroxidase-like nanozymes for the rapid, low-cost, on-site detection of TAC. The pristine SrMOF functioned as a peroxidase nanozyme, and its enzymatic activity was enhanced after doping it with Ce(IV) ions because of the multivalent nature and synergistic impact of the heteroatoms. The Ce-SrMOFs were sensitive to the single electron transfer and hydrogen atom transfer processes, which implies that the Ce-SrMOFs can serve as an ideal nanozyme candidate for TAC analysis. The investigated mechanism revealed that •OH is the most active oxygen species for the peroxidase-like activity. The Ce-SrMOFs exhibited a strong affinity for 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2, with K m values of 0.082 and 0.427 mM, which are 5.29- and 8.67-fold lower than those of horseradish peroxidase (HRP), respectively. The Ce-SrMOFs were used for the detection of ascorbic acid, cysteine, and glutathione, with limits of detection of 44, 53, and 512 nM, respectively. The proposed method proved effective in measuring the TAC in saliva samples from lung cancer patients, thereby yielding results with satisfactory precision and accuracy.</description><identifier>ISSN: 1944-8244</identifier><identifier>ISSN: 1944-8252</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.3c01007</identifier><identifier>PMID: 37072289</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>active oxygen species ; antioxidant activity ; Antioxidants ; ascorbic acid ; catalytic activity ; Cerium ; Colorimetry - methods ; cysteine ; electron transfer ; enzyme activity ; Functional Inorganic Materials and Devices ; glutathione ; Humans ; hydrogen ; Hydrogen Peroxide - analysis ; Lung Neoplasms ; Metal-Organic Frameworks ; oxidative stress ; Oxidoreductases ; Peroxidase ; Peroxidases ; saliva ; Smartphone</subject><ispartof>ACS applied materials & interfaces, 2023-05, Vol.15 (17), p.21239-21251</ispartof><rights>2023 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a363t-78ab8838c727957bb42d70bbaf5268b152f03e68ee0501735e302062f04725ef3</citedby><cites>FETCH-LOGICAL-a363t-78ab8838c727957bb42d70bbaf5268b152f03e68ee0501735e302062f04725ef3</cites><orcidid>0000-0002-6866-4116</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/acsami.3c01007$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsami.3c01007$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,778,782,2754,27063,27911,27912,56725,56775</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37072289$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Alshatteri, Azad H.</creatorcontrib><creatorcontrib>Ali, Gona K.</creatorcontrib><creatorcontrib>Omer, Khalid M.</creatorcontrib><title>Enhanced Peroxidase-Mimic Catalytic Activity via Cerium Doping of Strontium-Based Metal–Organic Frameworks with Design of a Smartphone-Based Sensor for On-Site Salivary Total Antioxidant Capacity Detection in Lung Cancer Patients</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>The development of artificial nanozymes with superior catalytic performance and excellent stability has been a long-standing objective for chemists. The total antioxidant capacity (TAC) is one of the most important bioanalytical measures of oxidative stress in the body. The present work aims to develop a smartphone-assisted visual detection sensor using cerium-doped strontium-based metal–organic frameworks (Ce-SrMOFs) as peroxidase-like nanozymes for the rapid, low-cost, on-site detection of TAC. The pristine SrMOF functioned as a peroxidase nanozyme, and its enzymatic activity was enhanced after doping it with Ce(IV) ions because of the multivalent nature and synergistic impact of the heteroatoms. The Ce-SrMOFs were sensitive to the single electron transfer and hydrogen atom transfer processes, which implies that the Ce-SrMOFs can serve as an ideal nanozyme candidate for TAC analysis. The investigated mechanism revealed that •OH is the most active oxygen species for the peroxidase-like activity. The Ce-SrMOFs exhibited a strong affinity for 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2, with K m values of 0.082 and 0.427 mM, which are 5.29- and 8.67-fold lower than those of horseradish peroxidase (HRP), respectively. The Ce-SrMOFs were used for the detection of ascorbic acid, cysteine, and glutathione, with limits of detection of 44, 53, and 512 nM, respectively. The proposed method proved effective in measuring the TAC in saliva samples from lung cancer patients, thereby yielding results with satisfactory precision and accuracy.</description><subject>active oxygen species</subject><subject>antioxidant activity</subject><subject>Antioxidants</subject><subject>ascorbic acid</subject><subject>catalytic activity</subject><subject>Cerium</subject><subject>Colorimetry - methods</subject><subject>cysteine</subject><subject>electron transfer</subject><subject>enzyme activity</subject><subject>Functional Inorganic Materials and Devices</subject><subject>glutathione</subject><subject>Humans</subject><subject>hydrogen</subject><subject>Hydrogen Peroxide - analysis</subject><subject>Lung Neoplasms</subject><subject>Metal-Organic Frameworks</subject><subject>oxidative stress</subject><subject>Oxidoreductases</subject><subject>Peroxidase</subject><subject>Peroxidases</subject><subject>saliva</subject><subject>Smartphone</subject><issn>1944-8244</issn><issn>1944-8252</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFksGO0zAQhiMEYpeFK0fkI1opxbGT2D2WdBeQuupKWc7RJJm0XhI72E6X3ngH3pALr4FLy94QB8vW6P9-_x5PFL1O6CyhLHkHjYNBzXhDE0rFk-g8madpLFnGnj6e0_QseuHcPaU5ZzR7Hp1xQQVjcn4e_brSW9ANtuQWrfmmWnAY36hBNaQAD_3eh9Oi8Wqn_J7sFJACrZoGsjSj0htiOlJ6a7QPtfh9gFtyg4H7-f3H2m5AB_rawoAPxn5x5EH5LVmiUxt9IIGUA1g_bo3GE1yidsaSLqy1jkvlkZTQqx3YPbkzwZgswl1_gmofIo7QHIIt0WMIaTRRmqymEKw4vMqSW_AKtXcvo2cd9A5fnfaL6PP11V3xMV6tP3wqFqsYeM59LCTUUnLZCCbmmajrlLWC1jV0GctlnWSsoxxziUgzmgieIaeM5qGaCpZhxy-it0ff0ZqvEzpfDco12Peg0Uyu4jSlXCZznv1XyiTlnFMuWJDOjtLGGucsdtVoVWjdvkpodZiD6jgH1WkOAvDm5D3VA7aP8r8fHwSXR0EAq3szWR268i-336U3wVs</recordid><startdate>20230503</startdate><enddate>20230503</enddate><creator>Alshatteri, Azad H.</creator><creator>Ali, Gona K.</creator><creator>Omer, Khalid M.</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>7X8</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0002-6866-4116</orcidid></search><sort><creationdate>20230503</creationdate><title>Enhanced Peroxidase-Mimic Catalytic Activity via Cerium Doping of Strontium-Based Metal–Organic Frameworks with Design of a Smartphone-Based Sensor for On-Site Salivary Total Antioxidant Capacity Detection in Lung Cancer Patients</title><author>Alshatteri, Azad H. ; Ali, Gona K. ; Omer, Khalid M.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a363t-78ab8838c727957bb42d70bbaf5268b152f03e68ee0501735e302062f04725ef3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>active oxygen species</topic><topic>antioxidant activity</topic><topic>Antioxidants</topic><topic>ascorbic acid</topic><topic>catalytic activity</topic><topic>Cerium</topic><topic>Colorimetry - methods</topic><topic>cysteine</topic><topic>electron transfer</topic><topic>enzyme activity</topic><topic>Functional Inorganic Materials and Devices</topic><topic>glutathione</topic><topic>Humans</topic><topic>hydrogen</topic><topic>Hydrogen Peroxide - analysis</topic><topic>Lung Neoplasms</topic><topic>Metal-Organic Frameworks</topic><topic>oxidative stress</topic><topic>Oxidoreductases</topic><topic>Peroxidase</topic><topic>Peroxidases</topic><topic>saliva</topic><topic>Smartphone</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Alshatteri, Azad H.</creatorcontrib><creatorcontrib>Ali, Gona K.</creatorcontrib><creatorcontrib>Omer, Khalid M.</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Alshatteri, Azad H.</au><au>Ali, Gona K.</au><au>Omer, Khalid M.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enhanced Peroxidase-Mimic Catalytic Activity via Cerium Doping of Strontium-Based Metal–Organic Frameworks with Design of a Smartphone-Based Sensor for On-Site Salivary Total Antioxidant Capacity Detection in Lung Cancer Patients</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl. Mater. Interfaces</addtitle><date>2023-05-03</date><risdate>2023</risdate><volume>15</volume><issue>17</issue><spage>21239</spage><epage>21251</epage><pages>21239-21251</pages><issn>1944-8244</issn><issn>1944-8252</issn><eissn>1944-8252</eissn><abstract>The development of artificial nanozymes with superior catalytic performance and excellent stability has been a long-standing objective for chemists. The total antioxidant capacity (TAC) is one of the most important bioanalytical measures of oxidative stress in the body. The present work aims to develop a smartphone-assisted visual detection sensor using cerium-doped strontium-based metal–organic frameworks (Ce-SrMOFs) as peroxidase-like nanozymes for the rapid, low-cost, on-site detection of TAC. The pristine SrMOF functioned as a peroxidase nanozyme, and its enzymatic activity was enhanced after doping it with Ce(IV) ions because of the multivalent nature and synergistic impact of the heteroatoms. The Ce-SrMOFs were sensitive to the single electron transfer and hydrogen atom transfer processes, which implies that the Ce-SrMOFs can serve as an ideal nanozyme candidate for TAC analysis. The investigated mechanism revealed that •OH is the most active oxygen species for the peroxidase-like activity. The Ce-SrMOFs exhibited a strong affinity for 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2, with K m values of 0.082 and 0.427 mM, which are 5.29- and 8.67-fold lower than those of horseradish peroxidase (HRP), respectively. The Ce-SrMOFs were used for the detection of ascorbic acid, cysteine, and glutathione, with limits of detection of 44, 53, and 512 nM, respectively. The proposed method proved effective in measuring the TAC in saliva samples from lung cancer patients, thereby yielding results with satisfactory precision and accuracy.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>37072289</pmid><doi>10.1021/acsami.3c01007</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0002-6866-4116</orcidid></addata></record> |
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subjects | active oxygen species antioxidant activity Antioxidants ascorbic acid catalytic activity Cerium Colorimetry - methods cysteine electron transfer enzyme activity Functional Inorganic Materials and Devices glutathione Humans hydrogen Hydrogen Peroxide - analysis Lung Neoplasms Metal-Organic Frameworks oxidative stress Oxidoreductases Peroxidase Peroxidases saliva Smartphone |
title | Enhanced Peroxidase-Mimic Catalytic Activity via Cerium Doping of Strontium-Based Metal–Organic Frameworks with Design of a Smartphone-Based Sensor for On-Site Salivary Total Antioxidant Capacity Detection in Lung Cancer Patients |
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