{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,10,12]],"date-time":"2025-10-12T04:34:36Z","timestamp":1760243676170,"version":"build-2065373602"},"reference-count":21,"publisher":"MDPI AG","issue":"6","license":[{"start":{"date-parts":[[2012,6,19]],"date-time":"2012-06-19T00:00:00Z","timestamp":1340064000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/3.0\/"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Sensors"],"abstract":"<jats:p>We fabricated an electrode chip with a structure coated by an insulation layer that contains dispersed SiO2 adsorbent particles modified by an amino-group on a source-drain electrode. Voltage changes caused by chelate molecule adsorption onto electrode surfaces and by specific cation interactions were investigated. The detection of specific cations without the presence of chelate molecules on the free electrode was also examined. By comparing both sets of results the complexation ability of the studied chelate molecules onto the electrode was evaluated. Five pairs of source-drain electrodes (\u00d78 arrays) were fabricated on a glass substrate of 20 \u00d7 30 mm in size. The individual Au\/Cr (1.0\/0.1 \u03bcm thickness) electrodes had widths of 50 \u03bcm and an inter-electrode interval of 100 \u03bcm. The fabricated source-drain electrodes were further coated with an insulation layer comprising a porous SiO2 particle modified amino-group to adsorb the chelate molecules. The electrode chip was equipped with a handy-type sensor signal analyzer that was mounted on an amplifier circuit using a MinishipTM or a system in a packaged LSI device. For electrode surfaces containing different adsorbed chelate molecules an increase in the sensor voltage depended on a combination of host-guest reactions and generally decreased in the following order: 5,10,15,20-tetrakis(N-methylpyridinium-4-yl)-21H,23H-porphine, tetrakis(p-toluenesulfonate) (TMPyP) as a Cu2+ chelator and Cu2+ &gt; 2-nitroso-5-[N-n-propyl-N-(3-sulfopropyl)amino]phenol (nitroso-PSAP) as an Fe2+ chelator and Fe2+ &gt; 4,7-diphenyl-1,10-phenanthrolinedisulfonic acid, disodium salt (BPDSA) as an Fe2+ chelator and Fe2+ &gt; 3-[3-(2,4-dimethylphenylcarbamoyl)-2-hydroxynaphthalene-1-yl-azo]-4-hydroxybenzenesulfonic acid, sodium salt (XB-1) as a Mg2+ chelator and Mg2+ &gt; 2,9-dimethyl-4,7-diphenyl-1,10-phenanthrolinedisulfonic acid, disodium salt (BCIDSA) as a Cu2+ chelator and Cu2+, respectively. In contrast, for the electrode surfaces with adsorbed O,O'-bis(2-aminoethyl)ethyleneglycol-N,N,N',N'-tetraacetic acid (GEDTA) or O,O'-bis(2-aminophenyl)ethyleneglycol-N,N,N',N'-tetraacetic acid, tetrapotassium salt, hydrate (BAPTA) as a Ca2+ chelator no increase in the detection voltage was found for all the electrode tests conducted in the presence of Ca2+. To determine the differences in electrode detection, molecular orbital (MO) calculations of the chelate molecules and surface molecular modeling of the adsorbents were carried out. In accordance with frontier orbital theory, the lowest unoccupied MO (LUMO) of the chelate molecules can accept two lone pair electrons at the highest occupied MO (HOMO) of the amino group on the model surface structure of the SiO2 particle. As a result, a good correlation was obtained between the LUMO-HOMO difference and the ion response of all the electrodes tested. Based on the results obtained, the order of adsorbed chelate molecules on adsorption particles reflects the different metal ion detection abilities of the electrode chips.<\/jats:p>","DOI":"10.3390\/s120608405","type":"journal-article","created":{"date-parts":[[2012,6,19]],"date-time":"2012-06-19T12:49:40Z","timestamp":1340110180000},"page":"8405-8425","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Evaluation of Complexation Ability Using a Sensor Electrode Chip Equipped with a Wireless Screening System"],"prefix":"10.3390","volume":"12","author":[{"given":"Takaaki","family":"Isoda","sequence":"first","affiliation":[{"name":"Department of Life and Environment Engineering, Faculty of Environmental Engineering, University of Kitakyushu, 1-1, Hibikino, Wakamatsu, Kitakyushu 808-0135, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Ikuko","family":"Urushibara","sequence":"additional","affiliation":[{"name":"AR\u2019S CO., Ltd., 5-1, Yokohama Creation Square, Sakaecho, Kanagawa, Yokohama 221-0052, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Hikaru","family":"Sato","sequence":"additional","affiliation":[{"name":"AR\u2019S CO., Ltd., 5-1, Yokohama Creation Square, Sakaecho, Kanagawa, Yokohama 221-0052, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Noriyoshi","family":"Yamauchi","sequence":"additional","affiliation":[{"name":"The Graduate School of Information, Production and Systems, Waseda University, 2-7, Hibikino, Wakamatsu, Kitakyushu 808-0135, Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"1968","published-online":{"date-parts":[[2012,6,19]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"538","DOI":"10.1016\/j.snb.2011.01.003","article-title":"Polymer-grafted QCM chemical sensor and application to heavy metal ions real time detection.Sens.","volume":"155","author":"Sartore","year":"2011","journal-title":"Actuators B"},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"7","DOI":"10.1016\/j.snb.2008.12.050","article-title":"8-OHdG Sensing with MIP based solid phase extraction and QCM technique","volume":"137","author":"Diltemiz","year":"2009","journal-title":"Sens. Actuators B"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"320","DOI":"10.1016\/j.snb.2007.08.007","article-title":"Surface modification of thin polyion complex film for surface plasmon resonance immunosensor","volume":"130","author":"Kurita","year":"2008","journal-title":"Sens. Actuators B"},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"494","DOI":"10.1016\/j.snb.2009.08.037","article-title":"A new compact electrochemical method for analyzing complex protein films adsorbed on the surface of modified interdigitated gold electrodes","volume":"142","author":"Hedlund","year":"2009","journal-title":"Sens. Actuators B"},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"203","DOI":"10.1016\/0925-4005(93)85052-C","article-title":"Amperometric determination of copper using screen-printed electrodes","volume":"15","author":"Somasundrum","year":"1993","journal-title":"Sens. Actuators B"},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"210","DOI":"10.1016\/j.snb.2007.11.004","article-title":"Phytase immobilization on modified electrodes for amperometric biosensing","volume":"131","author":"Moraes","year":"2008","journal-title":"Sens. Actuators B"},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"726","DOI":"10.1016\/j.snb.2010.01.027","article-title":"Chelating electrodes as taste sensor for the trace assessment of metal ions","volume":"145","author":"Heras","year":"2010","journal-title":"Sens. Actuators B"},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"488","DOI":"10.1016\/0925-4005(92)80349-3","article-title":"Multisensor array for pH, K+, Na+ and Ca2+measurements based on coated-film electrodes","volume":"7","author":"Lemke","year":"1992","journal-title":"Sens. Actuators B"},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"391","DOI":"10.1016\/j.snb.2006.08.043","article-title":"A MEMS fabricated cell electrophysiology biochip for in silico calcium measurements","volume":"123","author":"Haque","year":"2007","journal-title":"Sens. Actuators B"},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"958","DOI":"10.1016\/j.snb.2007.10.022","article-title":"Development of a sensor-array chip with immobilized antibodies and the application of a wireless antigen-screening system","volume":"129","author":"Isoda","year":"2008","journal-title":"Sens. Actuators B"},{"key":"ref_11","first-page":"237","article-title":"Evaluation of immunoglobulin sensing function by using of a fullerene-composite-polymer coated sensor electrode","volume":"23","author":"Isoda","year":"2011","journal-title":"Sens.Mater."},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"1","DOI":"10.1007\/BF00128336","article-title":"MOPAC: A semiempirical molecular orbital program","volume":"4","author":"Stewart","year":"1990","journal-title":"J. Comput. Aided Mol. Des."},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"722","DOI":"10.1063\/1.1700523","article-title":"A molecular orbital theory of reactivity in aromatic hydrocarbons","volume":"20","author":"Fukui","year":"1952","journal-title":"J. Chem. Phys."},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"117","DOI":"10.1016\/j.snb.2012.01.025","article-title":"Phenanthroline derivatives electrochemically grafted to glassy carbon for Cu(II) ion detection","volume":"166","author":"Oztekin","year":"2012","journal-title":"Sens. Actuators B"},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"1645","DOI":"10.1002\/elan.201100121","article-title":"Electrochemical determination of Cu(II) ions by 4-formylphenylboronic acid modified gold electrode","volume":"23","author":"Oztekin","year":"2011","journal-title":"Electroanalysis"},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"235","DOI":"10.1016\/S0925-4005(02)00193-4","article-title":"Magnesium-selective electrodes","volume":"86","author":"Gupta","year":"2002","journal-title":"Sens. Actuators B"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"340","DOI":"10.1016\/j.snb.2003.11.033","article-title":"PVC based dibenzo-18-crown-6 electrode for Ca(II) ions","volume":"99","author":"Kumar","year":"2004","journal-title":"Sens. Actuators B"},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"709","DOI":"10.1016\/S0925-4005(03)00571-9","article-title":"Development of a solid-state thick film calcium ion-selective electrode","volume":"96","author":"Wang","year":"2003","journal-title":"Sens. Actuators B"},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"223","DOI":"10.1016\/j.snb.2004.06.005","article-title":"Fe3+ion sensing characteristics of polydiphenylamine-electrochemical and spectroelectro-chemical analysis","volume":"105","author":"Suganandam","year":"2005","journal-title":"Sens. Actuators B"},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"812","DOI":"10.1016\/j.snb.2005.07.039","article-title":"A Zn-selective electrode based on N,N\u2032-bis(acetylacetone)ethylenediimine","volume":"114","author":"Gupta","year":"2006","journal-title":"Sens. Actuators B"},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"401","DOI":"10.1016\/j.snb.2004.06.038","article-title":"Zn(II)-ion-selective electrodes based on GeSe2-Sb2Se3-ZnSe glasses","volume":"106","author":"Vassilev","year":"2005","journal-title":"Sens. Actuators B"}],"container-title":["Sensors"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/1424-8220\/12\/6\/8405\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,11]],"date-time":"2025-10-11T21:50:52Z","timestamp":1760219452000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/1424-8220\/12\/6\/8405"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2012,6,19]]},"references-count":21,"journal-issue":{"issue":"6","published-online":{"date-parts":[[2012,6]]}},"alternative-id":["s120608405"],"URL":"https:\/\/doi.org\/10.3390\/s120608405","relation":{},"ISSN":["1424-8220"],"issn-type":[{"type":"electronic","value":"1424-8220"}],"subject":[],"published":{"date-parts":[[2012,6,19]]}}}