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Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications

Simona Ferraraccio, James Russell, Ben Newland, Paolo Bertoncello Orcid Logo

Electrochimica Acta, Volume: 483

Swansea University Authors: Simona Ferraraccio, James Russell, Paolo Bertoncello Orcid Logo

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Abstract

Enzymes-based electrochemical biosensors require the immobilisation of the enzymes on the electrode surfaces as well as their storage in aqueous environments to maintain the enzymatic activity. Herein, we described an enzyme-based electrochemiluminescence biosensor fabricated by incorporating oxidas...

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Published in: Electrochimica Acta
ISSN: 0013-4686
Published: Elsevier BV 2024
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Herein, we described an enzyme-based electrochemiluminescence biosensor fabricated by incorporating oxidase enzymes (horseradish peroxidase, HRP; glucose, GOx, lactate, LOx, and cholesterol oxidases, ChOx) within poly(ethylene glycol)diacrylate (PEGDA) cryogels, which retain their activity when stored in dry conditions. The redox reactions between the oxidase enzymes and their corresponding substrates produce hydrogen peroxide that can be detected in the presence of a layer of polyluminol deposited on the electrode surface. These oxidases PEG-based cryogels were characterized using cyclic voltammetry and electrochemiluminescence (ECL) to assess the redox reactions between the enzymes and the corresponding substrates. The proposed biosensors were characterised by good stability and repeatability with a calculated limit of detections (LODs) in the micromolar concentration range. The performances of PEG cryogels over the time evidenced the stability of the as-prepared materials up to 30 days in dry conditions, confirming good retention of the encapsulated enzymes. Furthermore, the biosensors were tested in the presence of interferent species showing good selectivity. Finally, these oxidases-PEG cryogels were tested in real samples (commercial contact lenses, artificial sweat and commercial milk) confirming the suitability of such material for the detection of hydrogen peroxide with calculated LoDs as 10.37 ± 0.4 µM for HRP/contact lenses liquid; 3.87 ± 0.3 µM for GOx/artificial sweat; 1.09 ± 0.6 µM for LOx/artificial sweat; and 6.59 ± 0.5 for ChOx/milk.</abstract><type>Journal Article</type><journal>Electrochimica Acta</journal><volume>483</volume><journalNumber/><paginationStart/><paginationEnd/><publisher>Elsevier BV</publisher><placeOfPublication/><isbnPrint/><isbnElectronic/><issnPrint>0013-4686</issnPrint><issnElectronic/><keywords>Electrochemiluminescence; Electropolymerization; Enzyme; Encapsulation; PEG-cryogel</keywords><publishedDay>10</publishedDay><publishedMonth>4</publishedMonth><publishedYear>2024</publishedYear><publishedDate>2024-04-10</publishedDate><doi>10.1016/j.electacta.2024.144007</doi><url/><notes>Data availability:Data will be made available on request.</notes><college>COLLEGE NANME</college><department>Chemical Engineering</department><CollegeCode>COLLEGE CODE</CollegeCode><DepartmentCode>CHEG</DepartmentCode><institution>Swansea University</institution><apcterm>SU Library paid the OA fee (TA Institutional Deal)</apcterm><funders>L.S.F. gratefully acknowledges financial support from the Knowledge Economy Skills PhD Scholarship (KESS2) under the Welsh Government's European Social Fund (ESF) convergence program for West Wales and the Valleys and Perpetuus Carbon Ltd. P.B. acknowledges the Institute for Innovative Materials, Processing and Numerical Technologies (IMPACT) for the purchase of the ECL setup. The microscoscopic characterization was possible throughout the Advanced Imaging of Materials (AIM) facility (EPSRC Grant No. EP/M028267/1), the European Social Fund (ESF) through the European Union's Convergence programme administered by the Welsh Government (80708), and the Welsh Government Enhancing Competitiveness Grant (MA/KW/5554/19).</funders><projectreference/><lastEdited>2024-03-25T12:56:19.8349427</lastEdited><Created>2024-02-28T15:20:53.0812909</Created><path><level id="1">Faculty of Science and Engineering</level><level id="2">School of Engineering and Applied Sciences - Chemical Engineering</level></path><authors><author><firstname>Simona</firstname><surname>Ferraraccio</surname><order>1</order></author><author><firstname>James</firstname><surname>Russell</surname><orcid/><order>2</order></author><author><firstname>Ben</firstname><surname>Newland</surname><order>3</order></author><author><firstname>Paolo</firstname><surname>Bertoncello</surname><orcid>0000-0002-6557-7885</orcid><order>4</order></author></authors><documents><document><filename>65714__29827__ed6d628198424a9aaebbf49de92698c9.pdf</filename><originalFilename>65714.VOR.pdf</originalFilename><uploaded>2024-03-25T12:54:31.2947889</uploaded><type>Output</type><contentLength>7516158</contentLength><contentType>application/pdf</contentType><version>Version of Record</version><cronfaStatus>true</cronfaStatus><documentNotes>© 2024 The Author(s). 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spelling v2 65714 2024-02-28 Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications 1300f1211abc29e989f5aee998831070 Simona Ferraraccio Simona Ferraraccio true false 4ad47527c475ae228d69747c0c21f148 James Russell James Russell true false ad352842aa5fe9c1947bd24ff61816c8 0000-0002-6557-7885 Paolo Bertoncello Paolo Bertoncello true false 2024-02-28 CHEG Enzymes-based electrochemical biosensors require the immobilisation of the enzymes on the electrode surfaces as well as their storage in aqueous environments to maintain the enzymatic activity. Herein, we described an enzyme-based electrochemiluminescence biosensor fabricated by incorporating oxidase enzymes (horseradish peroxidase, HRP; glucose, GOx, lactate, LOx, and cholesterol oxidases, ChOx) within poly(ethylene glycol)diacrylate (PEGDA) cryogels, which retain their activity when stored in dry conditions. The redox reactions between the oxidase enzymes and their corresponding substrates produce hydrogen peroxide that can be detected in the presence of a layer of polyluminol deposited on the electrode surface. These oxidases PEG-based cryogels were characterized using cyclic voltammetry and electrochemiluminescence (ECL) to assess the redox reactions between the enzymes and the corresponding substrates. The proposed biosensors were characterised by good stability and repeatability with a calculated limit of detections (LODs) in the micromolar concentration range. The performances of PEG cryogels over the time evidenced the stability of the as-prepared materials up to 30 days in dry conditions, confirming good retention of the encapsulated enzymes. Furthermore, the biosensors were tested in the presence of interferent species showing good selectivity. Finally, these oxidases-PEG cryogels were tested in real samples (commercial contact lenses, artificial sweat and commercial milk) confirming the suitability of such material for the detection of hydrogen peroxide with calculated LoDs as 10.37 ± 0.4 µM for HRP/contact lenses liquid; 3.87 ± 0.3 µM for GOx/artificial sweat; 1.09 ± 0.6 µM for LOx/artificial sweat; and 6.59 ± 0.5 for ChOx/milk. Journal Article Electrochimica Acta 483 Elsevier BV 0013-4686 Electrochemiluminescence; Electropolymerization; Enzyme; Encapsulation; PEG-cryogel 10 4 2024 2024-04-10 10.1016/j.electacta.2024.144007 Data availability:Data will be made available on request. COLLEGE NANME Chemical Engineering COLLEGE CODE CHEG Swansea University SU Library paid the OA fee (TA Institutional Deal) L.S.F. gratefully acknowledges financial support from the Knowledge Economy Skills PhD Scholarship (KESS2) under the Welsh Government's European Social Fund (ESF) convergence program for West Wales and the Valleys and Perpetuus Carbon Ltd. P.B. acknowledges the Institute for Innovative Materials, Processing and Numerical Technologies (IMPACT) for the purchase of the ECL setup. The microscoscopic characterization was possible throughout the Advanced Imaging of Materials (AIM) facility (EPSRC Grant No. EP/M028267/1), the European Social Fund (ESF) through the European Union's Convergence programme administered by the Welsh Government (80708), and the Welsh Government Enhancing Competitiveness Grant (MA/KW/5554/19). 2024-03-25T12:56:19.8349427 2024-02-28T15:20:53.0812909 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Simona Ferraraccio 1 James Russell 2 Ben Newland 3 Paolo Bertoncello 0000-0002-6557-7885 4 65714__29827__ed6d628198424a9aaebbf49de92698c9.pdf 65714.VOR.pdf 2024-03-25T12:54:31.2947889 Output 7516158 application/pdf Version of Record true © 2024 The Author(s). This is an open access article under the CC BY license. true eng http://creativecommons.org/licenses/by/4.0/
title Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
spellingShingle Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
Simona Ferraraccio
James Russell
Paolo Bertoncello
title_short Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
title_full Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
title_fullStr Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
title_full_unstemmed Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
title_sort Poly(ethylene glycol)(PEG)-cryogels: A novel platform towards enzymatic electrochemiluminescence (ECL)-based sensor applications
author_id_str_mv 1300f1211abc29e989f5aee998831070
4ad47527c475ae228d69747c0c21f148
ad352842aa5fe9c1947bd24ff61816c8
author_id_fullname_str_mv 1300f1211abc29e989f5aee998831070_***_Simona Ferraraccio
4ad47527c475ae228d69747c0c21f148_***_James Russell
ad352842aa5fe9c1947bd24ff61816c8_***_Paolo Bertoncello
author Simona Ferraraccio
James Russell
Paolo Bertoncello
author2 Simona Ferraraccio
James Russell
Ben Newland
Paolo Bertoncello
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container_title Electrochimica Acta
container_volume 483
publishDate 2024
institution Swansea University
issn 0013-4686
doi_str_mv 10.1016/j.electacta.2024.144007
publisher Elsevier BV
college_str Faculty of Science and Engineering
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hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str 1
active_str 0
description Enzymes-based electrochemical biosensors require the immobilisation of the enzymes on the electrode surfaces as well as their storage in aqueous environments to maintain the enzymatic activity. Herein, we described an enzyme-based electrochemiluminescence biosensor fabricated by incorporating oxidase enzymes (horseradish peroxidase, HRP; glucose, GOx, lactate, LOx, and cholesterol oxidases, ChOx) within poly(ethylene glycol)diacrylate (PEGDA) cryogels, which retain their activity when stored in dry conditions. The redox reactions between the oxidase enzymes and their corresponding substrates produce hydrogen peroxide that can be detected in the presence of a layer of polyluminol deposited on the electrode surface. These oxidases PEG-based cryogels were characterized using cyclic voltammetry and electrochemiluminescence (ECL) to assess the redox reactions between the enzymes and the corresponding substrates. The proposed biosensors were characterised by good stability and repeatability with a calculated limit of detections (LODs) in the micromolar concentration range. The performances of PEG cryogels over the time evidenced the stability of the as-prepared materials up to 30 days in dry conditions, confirming good retention of the encapsulated enzymes. Furthermore, the biosensors were tested in the presence of interferent species showing good selectivity. Finally, these oxidases-PEG cryogels were tested in real samples (commercial contact lenses, artificial sweat and commercial milk) confirming the suitability of such material for the detection of hydrogen peroxide with calculated LoDs as 10.37 ± 0.4 µM for HRP/contact lenses liquid; 3.87 ± 0.3 µM for GOx/artificial sweat; 1.09 ± 0.6 µM for LOx/artificial sweat; and 6.59 ± 0.5 for ChOx/milk.
published_date 2024-04-10T12:56:16Z
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