ࡱ> BD123456789:;<=>?@A xbjbj̵ XPצצ.c&%%%%8]9%m8"===lllllllomr^l=M7===l L mN L L L= g L=l L LV$T@hTAghaei787817Aghaei, A.Hosseini, M. R. M.Najafi, M.A novel capacitive biosensor for cholesterol assay that uses an electropolymerized molecularly imprinted polymerElectrochimica ActaElectrochimica ActaElectrochim. Acta1503-1508555Feb0013-4686ISI:000275596900001<Go to ISI>://000275596900001 Zine2006797917Zine, N.Bausells, J.Vocanson, F.Lamartine, R.Asfari, Z.Teixidor, F.Crespo, E.de Oliveira, I. A. M.Samitier, J.Errachid, A.Potassium-ion selective solid contact microelectrode based on a novel 1,3-(di-4-oxabutanol)-calix[4]arene-crown-5 neutral carrierElectrochimica ActaElectrochimica ActaElectrochim. Acta5075-507951242006Jul0013-4686ISI:000239253900009<Go to ISI>://000239253900009 [1, 2], but also on the engineering of new sensing instrumentation and on how the information is retrieved  ADDIN EN.CITE Yang2009444417Yang, L.Zhang, R. W.Staiculescu, D.Wong, C. P.Tentzeris, M. M.A Novel Conformal RFID-Enabled Module Utilizing Inkjet-Printed Antennas and Carbon Nanotubes for Gas-Detection ApplicationsIeee Antennas and Wireless Propagation LettersIeee Antennas and Wireless Propagation Letters653-656820091536-1225ISI:000268020000046<Go to ISI>://000268020000046 Kim2008454517Kim, Y.Evans, R. G.Iversen, W. M.Remote sensing and control of an irrigation system using a distributed wireless sensor networkIeee Transactions on Instrumentation and MeasurementIeee Transactions on Instrumentation and Measurement1379-13875772008Jul0018-9456ISI:000256584800014<Go to ISI>://000256584800014 [3, 4]. The development of new sensing materials seems to be based on the use of single molecular probes capable of simultaneous determination of multianalytes  ADDIN EN.CITE Kaur2007383817Kaur, N.Kumar, S.Guru Nanak Dev Univ, Dept Chem, Amritsar 143005, Punjab, India. Kumar, S, Guru Nanak Dev Univ, Dept Chem, Amritsar 143005, Punjab, India. subodh_gndu@yahoo.co.inSingle molecular colorimetric probe for simultaneous estimation of Cu2+ and Ni2+Chemical CommunicationsChem. Commun.Chemical Communications3069-307029MULTIANALYTE SENSORMETAL-CATIONSRECOGNITIONQUANTIFICATIONANIONSARRAYS20071359-7345ISI:000248157100013Article<Go to ISI>://000248157100013 Kaur2008393917Kaur, N.Kumar, S.[Kaur, Navneet; Kumar, Subodh] Guru Nanak Dev Univ, Dept Chem, Amritsar 143005, Punjab, India. Kumar, S, Guru Nanak Dev Univ, Dept Chem, Amritsar 143005, Punjab, India. subodh_gndu@yahoo.co.inA differential receptor for selective and quantitative multi-ion analysis for Co2+ and Ni2+/Cu2+Tetrahedron LettersTetrahedron Lett.Tetrahedron Letters5067-50694934LARGE RED-SHIFTFLUORESCENT CHEMOSENSORMULTIANALYTE SENSORMETAL-CATIONSCOLOR CHANGESRECOGNITIONDEPROTONATIONSWITCHESQUANTIFICATIONLUMINESCENT2008Aug0040-4039ISI:000258271400022Article<Go to ISI>://000258271400022 [5, 6], and also on simultaneous detection via multiple detection channels inherent to the material studied  ADDIN EN.CITE Jimenez2005282817Jimenez, D.Martinez-Manez, R.Sancenon, F.Ros-Lis, J. V.Soto, J.Benito, A.Garcia-Breijo, E.Multi-channel receptors and their relation to guest chemosensing and reconfigurable molecular logic gatesEuropean Journal of Inorganic ChemistryEuropean Journal of Inorganic Chemistry2393-2403122005Jun1434-1948ISI:000230068200015<Go to ISI>://000230068200015 Jimenez2004272717Jimenez, D.Martinez-Manez, R.Sancenon, F.Soto, J.Electro-optical triple-channel sensing of metal cations via multiple signalling patternsTetrahedron LettersTetrahedron Letters1257-12594562004Feb0040-4039ISI:000188536900035<Go to ISI>://000188536900035 Andria737317Andria, S. E.Seliskar, C. J.Heineman, W. R.Simultaneous Detection of Two Analytes Using a Spectroelectrochemical SensorAnalytical ChemistryAnalytical Chemistry1720-1726825Mar0003-2700ISI:000274841300027<Go to ISI>://000274841300027 [7-9]. At the same time, the instrument used for detection should be non-invasive on the sample, and be capable of performing multiple analyses in a short space of time. Combining these efforts represents an obvious incentive to improve many aspects of chemical sensing, such as in the remote, autonomous monitoring of analytes  ADDIN EN.CITE Cleary2008535317Cleary, J.Slater, C.McGraw, C.Diamond, D.An autonomous microfluidic sensor for phosphate: On-site analysis of treated wastewaterIeee Sensors JournalIeee Sensors Journal508-51585-62008May-Jun1530-437XISI:000258763200013<Go to ISI>://000258763200013 McGraw2007545417McGraw, C. M.Stitzel, S. E.Cleary, J.Slater, C.Diamond, D.Autonomous microfluidic system for phosphate detectionTalantaTalanta1180-11857132007Feb0039-9140ISI:000244536800027<Go to ISI>://000244536800027 [10, 11]. Ionic Liquids (ILs) exhibit both a negligible vapour pressure and a wide electrochemical window  ADDIN EN.CITE Galinski2006626217Galinski, M.Lewandowski, A.Stepniak, I.Ionic liquids as electrolytesElectrochimica ActaElectrochimica ActaElectrochim. Acta5567-558051262006Aug0013-4686ISI:000240167400001<Go to ISI>://000240167400001 [12], and have emerged as quite promising materials in both electrochemistry  ADDIN EN.CITE Zhao2008555517Zhao, C.Burrell, G.Torriero, A. A. J.Separovic, F.Dunlop, N. F.MacFarlane, D. R.Bond, A. M.Electrochemistry of room temperature protic ionic liquidsJournal of Physical Chemistry BJournal of Physical Chemistry B6923-6936112232008Jun1520-6106ISI:000256492300005<Go to ISI>://000256492300005 Armand2009232317Armand, M.Endres, F.MacFarlane, D. R.Ohno, H.Scrosati, B.Ionic-liquid materials for the electrochemical challenges of the futureNature MaterialsNature Materials621-629882009Aug1476-1122ISI:000268288000012<Go to ISI>://000268288000012 [13, 14] and electrochemical sensing  ADDIN EN.CITE Yang646417Yang, M. H.Choi, B. G.Park, H.Hong, W. H.Lee, S. Y.Park, T. J.Development of a Glucose Biosensor Using Advanced Electrode Modified by Nanohybrid Composing Chemically Modified Graphene and Ionic LiquidElectroanalysisElectroanalysis1223-12282211Jun1040-0397ISI:000278850200010<Go to ISI>://000278850200010 [15]. ILs are the product of an ion-exchange metathesis reaction, resulting in a unique combination of ions that are liquid at room temperature  ADDIN EN.CITE Fraser2009616117Fraser, K. J.MacFarlane, D. R.Phosphonium-Based Ionic Liquids: An OverviewAustralian Journal of ChemistryAustralian Journal of Chemistry309-32162420090004-9425ISI:000265477900004<Go to ISI>://000265477900004 Chiappe2005636317Chiappe, C.Pieraccini, D.Ionic liquids: solvent properties and organic reactivityJournal of Physical Organic ChemistryJournal of Physical Organic Chemistry275-2971842005Apr0894-3230ISI:000227926800001<Go to ISI>://000227926800001 [16, 17]. They may find use in virtually all branches of chemistry, most notably as alternative non-volatile solvents in organic synthesis  ADDIN EN.CITE Chowdhury2007606017Chowdhury, S.Mohan, R. S.Scott, J. L.Reactivity of ionic liquidsTetrahedronTetrahedron2363-238963112007Mar0040-4020ISI:000244732800001<Go to ISI>://000244732800001 [18] but also fulfilling the same role in ionic polymeric based transducers  ADDIN EN.CITE Bennett2004131317Bennett, M. D.Leo, D. J.Ionic liquids as stable solvents for ionic polymer transducersSensors and Actuators a-PhysicalSensors and Actuators a-Physical79-9011512004Sep0924-4247ISI:000223611000013<Go to ISI>://000223611000013 Bennett2006121217Bennett, M. D.Leo, D. J.Wilkes, G. L.Beyer, F. L.Pechar, T. W.A model of charge transport and electromechanical transduction in ionic liquid-swollen Nafion membranesPolymerPolymer6782-679647192006Sep0032-3861ISI:000241171800039<Go to ISI>://000241171800039 [19, 20]. Conversely ILs have been studied as co-ordinating media, with complexes of most transition and some lanthanide metals reported  ADDIN EN.CITE Mehdi353517Mehdi, H.Binnemans, K.Van Hecke, K.Van Meervelt, L.Nockemann, P.[Mehdi, Hasan; Binnemans, Koen; Van Hecke, Kristof; Van Meervelt, Luc; Nockemann, Peter] Katholieke Univ Leuven, Dept Chem, B-3001 Heverlee, Belgium. Binnemans, K, Katholieke Univ Leuven, Dept Chem, Celestijnenlaan 200F Bus 2404, B-3001 Heverlee, Belgium. Koen.Binnemans@chem.kuleuven.be P.Nockemann@qub.ac.ukHydrophobic ionic liquids with strongly coordinating anionsChemical CommunicationsChem. Commun.Chemical Communications234-236462CARBON-DIOXIDEBETA-DIKETONESEXTRACTION1359-7345ISI:000272799200010Article<Go to ISI>://000272799200010 Nockemann363617Nockemann, P.Pellens, M.Van Hecke, K.Van Meervelt, L.Wouters, J.Thijs, B.Vanecht, E.Parac-Vogt, T. N.Mehdi, H.Schaltin, S.Fransaer, J.Zahn, S.Kirchner, B.Binnemans, K.Cobalt(II) Complexes of Nitrile-Functionalized Ionic LiquidsChemistry-a European JournalChemistry-a European Journal1849-18581660947-6539ISI:000275240300019<Go to ISI>://000275240300019 Lunstroot2009373717Lunstroot, K.Driesen, K.Nockemann, P.Van Hecke, K.Van Meervelt, L.Gorller-Walrand, C.Binnemans, K.Bellayer, S.Viau, L.Le Bideau, J.Vioux, A.Lanthanide-doped luminescent ionogelsDalton TransactionsDalton Transactions298-306220091477-9226ISI:000261807400011<Go to ISI>://000261807400011 [21-23]. Furthermore, the ease of incorporation of ILs into a polymer support (most commonly via in situ polymerisation of the monomer dissolved in the IL  ADDIN EN.CITE Ueki2008517517Ueki, T.Watanabe, M.Macromolecules in ionic liquids: Progress, challenges, and opportunitiesMacromoleculesMacromolecules3739-374941112008Jun0024-9297ISI:000256393500001<Go to ISI>://000256393500001 [24] or via polymer swelling  ADDIN EN.CITE Izak2007747417Izak, P.Hovorka, S.Bartovsky, T.Bartovska, L.Crespo, J. G.Swelling of polymeric membranes in room temperature ionic liquidsJournal of Membrane ScienceJournal of Membrane Science131-1382961-22007Jun0376-7388ISI:000246988800016<Go to ISI>://000246988800016 [25]) provides the basis for both solid state electrolyte  ADDIN EN.CITE Gayet767617Gayet, F.Viau, L.Leroux, F.Monge, S.Robin, J. J.Vioux, A.Polymer nanocomposite ionogels, high-performance electrolyte membranesJournal of Materials ChemistryJournal of Materials Chemistry9456-946220420959-9428ISI:000283264500022<Go to ISI>://000283264500022 Armel2011818117Armel, V.Velayutham, D.Sun, J. Z.Howlett, P. C.Forsyth, M.MacFarlane, D. R.Pringle, J. M.Ionic liquids and organic ionic plastic crystals utilizing small phosphonium cationsJournal of Materials ChemistryJournal of Materials Chemistry7640-7650212120110959-9428ISI:000290670000018<Go to ISI>://000290670000018 Sutto2011828217Sutto, T. E.Duncan, T. T.Wong, T. C.McGrady, K.Ionic liquid batteries: Chemistry to replace alkaline/acid energy storage devicesElectrochimica ActaElectrochimica ActaElectrochim. Acta3375-33795692011Mar0013-4686ISI:000290084700038<Go to ISI>://000290084700038 [26-28] and sensing templates  ADDIN EN.CITE Yang777717Yang, S. Y.Cicoira, F.Byrne, R.Benito-Lopez, F.Diamond, D.Owens, R. M.Malliaras, G. G.Electrochemical transistors with ionic liquids for enzymatic sensingChemical CommunicationsChemical Communications7972-797446421359-7345ISI:000283260400030<Go to ISI>://000283260400030 [29]. Our technique for the production of IL based polymer membranes involves the co-dissolution of the IL and polyvinylchloride (PVC) with Tetrahydrofuran (THF). As the solvent completely evaporates over time (12h) a transparent polymer film is produced (see experimental section). In our previous work we described how the many favourable properties of the IL trihexyltetradecylphosphonium dicyanamide [P6,6,6,14][DCA] was incorporated into polymeric based optodes. [P6,6,6,14][DCA] acted as ion-exchanger, plasticizer, ligand and colorimetric dye in PVC based membranes, these membranes produced an optical response upon exposure to Cu2+ (yellow), Co2+ (blue) and both ions simultaneously (green)  ADDIN EN.CITE Kavanagh808017Kavanagh, A.Byrne, R.Diamond, D.Radu, A.A two-component polymeric optode membrane based on a multifunctional ionic liquidAnalystAnalyst348-353136220100003-2654ISI:000285513000019<Go to ISI>://000285513000019 [30]. We now wish to expand on the use of ILs in polymeric membrane based sensors capable of generating optical and electrochemical signal responses. The Wireless Radio Frequency (WRF) detection instrument used in this study works particularly well for solid state, conductive samples. A signal is produced that is a direct function of the ability of the solid material to facilitate an electrical conductivity through ion movement. It has the required sensitivity, is non-invasive on the sample to be analysed and is capable of batch analyses in short spaces of time  ADDIN EN.CITE Clark20097717Clark, N. B.Maher, L. J.Non-contact, radio frequency detection of ammonia with a printed polyaniline sensorReactive & Functional PolymersReactive & Functional Polymers594-6006982009Aug1381-5148ISI:000268363500004<Go to ISI>://000268363500004 [31]. The goal of this work therefore is a proof of concept case intended to (a) exhibit 2-component polymeric optodes as electroactive materials capable of generating observable electrochemical signals as a result of transition metal ion binding; and (b) demonstrate and validate the use of WRF detection technology by varying both components of the polymeric membrane and monitoring their inherent ionic conductivity. The WRF instrument produces a signal in arbitrary units; its response has been validated principally by Electrochemical Impedance Spectroscopy (EIS). The level of ion coordination within the respective membrane has been characterised by X-Ray Fluorescence (XRF) Spectroscopy; which allows the reader to elucidate both observable trends in the WRF and EIS results. 3. Experimental 3.1 Chemicals and Materials Trihexyltetradecylphosphonium dicyanamide [P6,6,6,14][DCA] was generously donated by CYTEC industries. Further purification was achieved by washing with both water and hexane, and by column cleansing with basic alumina  ADDIN EN.CITE Ramnial2008686817Ramnial, T.Taylor, S. A.Bender, M. L.Gorodetsky, B.Lee, P. T. K.Dickie, D. A.McCollum, B. M.Pye, C. C.Walsby, C. J.Clyburne, J. A. C.Carbon-centered strong bases in phosphonium ionic liquidsJournal of Organic ChemistryJournal of Organic Chemistry801-8127332008Feb0022-3263ISI:000252686400004<Go to ISI>://000252686400004 [32]. Poly(vinyl)chloride (PVC), Poly(3-octylthiophene-2,5-diyl) (POT), Copper Nitrate trihydrate, Cobalt Nitrate hexahydrate, Aluminum oxide(activated, basic, Brockmann 1), Chloroform, Hexane and anhydrous Tetrahydrofuran (THF) were used as purchased from Sigma-Aldrich Ireland Ltd. 3.2 Polymer Membrane Preparation In order to prepare membranes; both PVC and [P6,6,6,14][DCA] in their respective ratios (totalling 240mg) were dissolved in 3mL of anhydrous THF and left to stir for 5 minutes until completely dissolved. Once dissolved the cocktail was then poured into a glass ring bound to a glass slide by rubber bands. They were then covered and left to dry overnight. The result is a clear, homogenous membrane of approximately 2.5cm in diameter and approximately 0.28mm in thickness. Once dry the membranes were then exposed to 1mL of a 0.1M metal ion solution for 12 hours. The metal salt solution was then removed by decanting of the liquid off the hydrophobic surface. The membrane was next dried in an oven overnight at 400C leaving the desired colour for analysis. 3.3 RF Wireless Conductivity Analysis All measurements were performed using the A PCIS-3000 10-95 6536 radio frequency detector (Detection Systems, Melbourne, Australia). All measurements were performed at 83.18 kHz, the speed of the carousel was kept at 8.9 metres per minute. The individual membranes to be analysed were initially cut to a 10 x 20mm strip. The film strip was then placed onto a non-conducting glass slide and placed inside the polystyrene container. In order to improve the accuracy of the reading, the strip was aligned vertically with the signal vector from the instrument. To further improve the accuracy of the measurement all samples were allowed to pass through the electrode channel 5 times. The response was analysed via peak area integration; which accounts for the contribution of the whole sample to the response obtained as well as the sample dimensions. The values quoted are normalised according to the sample weight; a detailed account of how the responses were obtained can be found in figure S1. The results of the data analysis are the values quoted below. 3.4 Electrochemical Impedance Spectroscopy Characterization was performed using the CHI Instruments 660A potentiostat. Screen-printed carbon paste silver electrodes with an active electrode area of 9mm2 were prepared in-house using a previously reported technique  ADDIN EN.CITE Morrin2003222217Morrin, A.Killard, A. J.Smyth, M. R.Electrochemical characterization of commercial and home-made screen-printed carbon electrodesAnalytical LettersAnalytical Letters2021-203936920030003-2719ISI:000184660600021<Go to ISI>://000184660600021 [33]. The electrodes were initially dropcast with a layer of POT (10-2M in chloroform) in order to aid the conversion of ionic to electronic conductivity in accordance with previous works  ADDIN EN.CITE Kavanagh2011838317Kavanagh, A.Copperwhite, R.Oubaha, M.Owens, J.McDonagh, C.Diamond, D.Byrne, R.Photo-patternable hybrid ionogels for electrochromic applicationsJournal of Materials ChemistryJournal of Materials Chemistry8687-8693212420110959-9428ISI:000291352900030<Go to ISI>://000291352900030 Bobacka2003848417Bobacka, J.Ivaska, A.Lewenstam, A.Potentiometric ion sensors based on conducting polymersElectroanalysisElectroanalysis366-374155-62003Apr1040-0397ISI:000182694800004<Go to ISI>://000182694800004 D. Cicmil2011515117D. Cicmil, S. Anastasova, A. Kavanagh, D. Diamond,U. Mattinen, J. Bobacka,A. Lewenstam and A. RaduIonic Liquid-Based, Liquid-Junction-Free Reference ElectrodeElectroanalysis&#xD;</secondary-title></titles><dates><year>2011</year></dates><urls></urls><electronic-resource-num>Analyst, DOI:10.1039/C0AN00770F.</electronic-resource-num></record></Cite></EndNote>[34-36]. 100L of the membrane cocktail composition (in 1mL THF) to be analysed was then dropcast onto the silver electrode using a 1mL microsyringe. The resultant dry membranes on the electrodes were then left in their respective metal ion salt solution overnight. The thickness of the resultant membranes were estimated using a Mitutoyo micrometer calibrated to a resolution of 1m. The impedance measurements were performed in the frequency range of 1 MHz to 0.01 Hz with a perturbation signal of 100mV. The reference electrode used was an aqueous Ag/AgCl (CHI Instruments 111, surface area: 3.14 mm2). A platinum wire electrode (CHI Instruments 115, surface area: 3.14 mm2) was used as the counter. A 1nF capacitance shunt was used to reduce high frequency noise. In order to obtain the impedance of the non-complexed membrane, the electrode in question was placed in 6ml of a 0.1M KCl solution. K+ is a soft, non-coordinating cation, and with no reported complexation behaviour with [DCA]-. 3.5 Portable XRF Measurements Measurements were performed using the Thermo NITON portable XRF analyser, using the standard thin film mode. In order to improve the accuracy of the measurement a batch reading of 3 x 180secs was performed. The averages of these measurements are the values quoted below. 4. Results and Discussion 4.1 Membrane Components Dicyanamide (DCA)- has previously been termed a pseudohalide with rather complex binding stoichiometry  ADDIN EN.CITE Batten2003696917Batten, S. R.Murray, K. S.Structure and magnetism of coordination polymers containing dicyanamide and tricyanomethanideCoordination Chemistry ReviewsCoordination Chemistry Reviews103-1302461-22003Nov0010-8545ISI:000187018300006<Go to ISI>://000187018300006 [37]. Complexation of this ligand with heavy metals results in net neutral complexes of 1, 2 and 3 dimensions  ADDIN EN.CITE Dong2003505017Dong, W.Liang, M.Sun, Y. Q.Liu, Z. Q.Nankai Univ, Dept Chem, Tianjin 300071, Peoples R China. Dong, W, Nankai Univ, Dept Chem, Tianjin 300071, Peoples R China. coord@nankai.edu.cnSyntheses and structures of two 1-D complexes, [Co(dmf)(2)(NCNCN)(2)] and [Cu(bipy)(NCNCN)]ClO4 with bridging dicyanamide ligandsZeitschrift Fur Anorganische Und Allgemeine ChemieZ. Anorg. Allg. Chem.Zeitschrift Fur Anorganische Und Allgemeine ChemieZ. Anorg. Allg. Chem.Zeitschrift Fur Anorganische Und Allgemeine ChemieZ. Anorg. Allg. Chem.2443-244562914coppercobaltdicyanamide bridgeMAGNETIC-PROPERTIESCRYSTAL-STRUCTURETEMPERATUREPOLYMERSANION2003Dec0044-2313ISI:000188203600007Article<Go to ISI>://000188203600007 Jones2006494917Jones, L. F.O'Dea, L.Offermann, D. A.Jensen, P.Moubaraki, B.Murray, K. S.Monash Univ, Sch Chem, Clayton, Vic 3800, Australia. Jones, LF, Monash Univ, Sch Chem, Clayton Campus,Bldg 23, Clayton, Vic 3800, Australia. leigh.jones@sci.monash.edu.au keith.murray@sci.monash.edu.auBenzotriazole based 1-D, 2-D and 3-D metal dicyanamide and tricyanomethanide coordination networksPolyhedronPolyhedronPolyhedronPolyhedronPolyhedronPolyhedron360-372252benzotriazolecoordination networksdicyanamidetricyanomethanidecrystal structuresmagnetismMAGNETIC-PROPERTIESX-RAYCOPOLYMERSDCANIN(CN)(2)(-)COMPLEXESLIGANDSFE2006Jan0277-5387ISI:000234928500021Article<Go to ISI>://000234928500021 [38, 39] plus electrochemically neutral co-ordinated polymers  ADDIN EN.CITE Manson1999686817Manson, J. L.Arif, A. M.Incarvito, C. D.Liable-Sands, L. M.Rheingold, A. L.Miller, J. S.Structures and magnetic properties of novel 1-D coordination polymers containing both dicyanamide and pyridine-type ligandsJournal of Solid State ChemistryJournal of Solid State Chemistry369-37814521999Jul0022-4596ISI:000081473200002<Go to ISI>://000081473200002 [40]. It was first used as an anion for ILs as its extensive electron delocalisation meant it only exhibited electrostatic interactions with the IL cation; resulting in a liquid with a comparably low viscosity ADDIN EN.CITE MacFarlane2001858517MacFarlane, D. R.Golding, J.Forsyth, S.Forsyth, M.Deacon, G. B.Low viscosity ionic liquids based on organic salts of the dicyanamide anionChemical CommunicationsChemical Communications1430-1431162001Aug1359-7345ISI:000170564800004<Go to ISI>://000170564800004 [41]. Solid, hydrophobic, polymeric membranes of this nature are typical of those used in Ion-Selective Electrodes (ISEs)  ADDIN EN.CITE Bakker1997202017Bakker, EricBuehlmann, PhilippePretsch, ErnoeCarrier-Based Ion-Selective Electrodes and Bulk Optodes. 1. General CharacteristicsChemical ReviewsChemical Reviews3083-3132978review ion selective electrode bulk optode1997An 1997:750190[42], a type of electrochemical sensor used for the determination of trace amounts of ions in solution. As the analysis typically involves the migration of an analyte between an aqueous phase and the hydrophobic polymeric surface, the mechanism of ion-transfer must be taken into account. In our previous work we have detailed that the migration mechanism of metal ions from aqueous to organic phase is co-extraction of the metal and its counter ion into the membrane rather than the ion-exchange convention [30]. In this case as the metal ion transfers through the polymeric membrane boundary it complexes and neutralises the anionic ligand; the counter ion of the metal salt (NO3) must therefore cross the membrane boundary in order to preserve electroneutrality within the membrane. The two principal components used in ISE membranes are the polymer and the plasticiser. Depending on the analytical approach, the w/w ratio of these can vary greatly, although a ratio of 2:1 plasticiser: polymer (w/w) is generally accepted as the optimum. Changing the IL-polymer ratio can significantly influence important characteristics such as physical stability and elasticity  ADDIN EN.CITE Shvedene2006181817Shvedene, N. V.Chernyshov, D. V.Khrenova, M. G.Formanovsky, A. A.Baulin, V. E.Pletnev, I. V.Moscow MV Lomonosov State Univ, Dept Chem, Moscow 119899, Russia. Russian Acad Sci, MM Shemyakin & Yu A Ovchinnikov Inst Bioorgan Che, Moscow 117997, Russia. Russian Acad Sci, Inst Physiol Act Cpds, Chernogolovka 142432, Russia. Pletnev, IV, Moscow MV Lomonosov State Univ, Dept Chem, GSP 3, Moscow 119899, Russia. pletnev@analyt.chem.msu.ruIonic liquids plasticize and bring ion-sensing ability to polymer membranes of selective electrodesElectroanalysisElectroanalysisElectroanalysisElectroanalysis1416-14211813-14ionic liquidsplasticized membranesion-selective electrodesMOLTEN-SALTSSOLVENT-EXTRACTIONTETRAFLUOROBORATECHROMATOGRAPHY2006Jul1040-0397ISI:000239380400022Proceedings Paper<Go to ISI>://000239380400022 [43]. In order to elucidate what affect the ratio of components will impart on the resulting conductivity and binding levels, the amounts of [P6,6,6,14][DCA] were varied from 66wt% to 50wt% and 33wt%. The characteristics of the resulting membranes were then investigated using WRF, EIS and XRF. 4.2 Membrane Component Ratio 2:1, IL:PVC. The WRF detector system used in this study utilises radio frequency technology in order to obtain the conductivity of a sample as it passes through a defined point. This point is the transmitting electrode, which passes a low voltage, low-frequency AC signal toward a receiving electrode wirelessly. The sample to be analysed is housed in an insulating polystyrene based container which is placed on a miniature conveyor (Fig 1). The insulating container with the sample placed inside is then allowed to pass through the electrode channel where it is processed and analysed via a PC. It has been used to great effect previously for the wireless detection of acetic acid and ammonia vapour using ink-jet printed polyaniline dispersions  ADDIN EN.CITE Clark20097717Clark, N. B.Maher, L. J.Non-contact, radio frequency detection of ammonia with a printed polyaniline sensorReactive & Functional PolymersReactive & Functional Polymers594-6006982009Aug1381-5148ISI:000268363500004<Go to ISI>://000268363500004 [31]. Figure 2 shows results obtained for a set of membranes containing a component ratio of 2:1, IL: PVC. Firstly a blank membrane (i.e. no metal ion exposure) was allowed to pass through the electrode channel. Next, three membranes individually exposed to (a) Cu2+, (b) Co2+ and finally (c) a solution containing a mixture of both ions were then allowed to pass through the electrode channel. One can see from Figure 2 the response obtained for the blank membrane (bold, dashed line). It demonstrates that this membrane is indeed electroactive (due to the presence of the IL) as the WRF instrument proved capable of detecting it as it passed through the electrode channel. What is also interesting to observe is the signal reduction seen for the respective co-ordinated membranes, which ultimately means that they have become less conductive. This downward trend is most likely due to the co-ordinating chemistry of [DCA]-; as previously discussed. The observed signal trend is Cobalt > Mix > Copper which we believe is directly related to the level of ion transfer and co-ordination within the membrane; which will be discussed later in this text. Some features inherent to this technique are so called edge effects which occur as the sample container first enters and leaves the electrode channel. These signals occur as the dielectric constant of the insulating housing material changes upon initial and final contact with the voltage vector. This, coupled with the signal produced from the conductive strip, means that the graph obtained is an effective picture of the dimensions of the container as it passes through the channel, with the conductive sample housed safely inside. A summary of the peak area integration analysis can be seen below (table 1) and in figure S2. WRF detection is a novel technique producing peak heights of arbitrary units, and therefore its results must be validated appropriately. For this purpose, Electrochemical Impedance Spectroscopy (EIS) was employed, as this provides an independent estimation of the sample conductivity in S/cm. The resulting x-axis intercept of the Nyquist plot (fig 3.) is used to determine the resistance of charge transfer (RCT) of the membrane, which is then easily converted to the corresponding conductivity via the equations:  EMBED Equation.3  (1)  EMBED Equation.3  (2) where G is the conductance, R is the resistance,  is the conductivity, A is the cross sectional area of the working electrode and L is the estimated thickness of the polymer membrane on the electrode  ADDIN EN.CITE <EndNote><Cite><Author>Stallworth</Author>1999141417Stallworth, P. E.Fontanella, J. J.Wintersgill, M. C.Scheidler, C. D.Immel, J. J.Greenbaum, S. G.Gozdz, A. S.NMR, DSC and high pressure electrical conductivity studies of liquid and hybrid electrolytesJournal of Power SourcesJournal of Power Sources739-747811999Sep0378-7753ISI:000084090300141<Go to ISI>://000084090300141 Neves727217Neves, L. A.Benavente, J.Coelhoso, I. M.Crespo, J. G.Design and characterisation of Nafion membranes with incorporated ionic liquids cationsJournal of Membrane ScienceJournal of Membrane Science42-523471-2Feb0376-7388ISI:000273662200006<Go to ISI>://000273662200006 [44, 45]. Our screen printed, in-house electrodes have a cross sectional area of 9mm2  ADDIN EN.CITE Morrin2003222217Morrin, A.Killard, A. J.Smyth, M. R.Electrochemical characterization of commercial and home-made screen-printed carbon electrodesAnalytical LettersAnalytical Letters2021-203936920030003-2719ISI:000184660600021<Go to ISI>://000184660600021 [33]. In order to estimate the average thickness of the membrane; a Mitutoyo micrometer calibrated to a resolution of 1m was used. The results of the thickness analysis across 6 electrodes can be seen in figures S3-S5. Table 2 provides a summary of the results obtained. One can see from both figure 3 and table 2 that the impedance of the metal ion co-ordinated membranes has increased. Here the trend is inverted from the previous result obtained. In order to see how the response from the two instruments correlate, plots of both % decrease (WRF) and % increase (EIS) of the signal response vs. the samples were constructed (Figure S6). Both trends are effectively linear and complement each other. EIS is therefore an effective validation of the novel WRF instrumental result; whilst also providing an independent estimation the increase in response seen. We believe that the inverse trends seen must be related to the level of co-ordination within the membrane. In order to confirm this; XRF was then finally used. We have also seen previously in our optical characterisation that whilst [P6, 6, 6, 14] [DCA] is capable of binding to both Co2+ and Cu2+, its preferentiality is toward Cu2+. Again for this analysis, membranes containing the same component ratio were analysed and the metal salt solutions concentration were also kept constant. Figure 4 (above) depicts the spectra obtained; the first feature to note is that the peak height obtained for chlorine is approximately the same for all 4 membranes. This illustrates that the ratio of PVC is indeed kept constant for all measurements, and so acts as an internal standard. The peaks for both Cobalt and Copper are also labelled, it can be seen that the peak height is considerably higher for Copper over Cobalt, which is indicative of the binding preferentiality of the IL. The peak heights obtained for the mixture are also labelled; they are, of course lower than those obtained for the pure ion solutions. The reduction in peak height is more dramatic for Cobalt over Copper, and given that the initial metal salt solution contained a volume ratio of 2:1, Co2+:Cu2+, further strengthens our binding preferentiality argument. Not unlike its instrumental equivalent, the portable XRF analyser is also capable of quantifying the intensity of the fluorescent peak levels into parts per million concentrations (ppm)  ADDIN EN.CITE Hosseini2003676717Hosseini, S. H.Entezami, A. A.Conducting polymer blends of polypyrrole with polyvinyl acetate, polystyrene, and polyvinyl chloride based toxic gas sensorsJournal of Applied Polymer ScienceJournal of Applied Polymer Science49-629012003Oct0021-8995ISI:000184515100006<Go to ISI>://000184515100006 Vazquez20014417Vazquez, M.Mikhelson, K.Piepponen, S.Rama, J.Sillanpaa, M.Ivaska, A.Lewenstam, A.Bobacka, J.Determination of Na+, K+, Ca2+, and Cl- ions in wood pulp suspension using ion-selective electrodesElectroanalysisElectroanalysis1119-112413132001Sep1040-0397ISI:000171267200010<Go to ISI>://000171267200010 [46, 47]. The calculation is based on many factors, but is most heavily dependent on the weight fraction of the element in the membrane and the dimensions of the sample  ADDIN EN.CITE Beckhoff200665656B. BeckhoffHandbook of Practical X-Ray Fluorescence Analysis3092006Springer[48]. The quantitative results of the first set of XRF analyses are detailed in table 2. From this table it is easy to deduce that even though all of the membranes were exposed to the same concentration of metal ion solution, that the uptake of Copper is significantly higher than Cobalt (~2.2 times greater). 4.3 Membrane Component Ratio 1:1, IL:PVC. Increasing the amount of polymer in the membrane to 50wt% led to membranes with slightly reduced flexibility and elasticity. The polymer can also be viewed as an insulating matrix, so the resulting measured impedance should also increase; whilst the wireless conductivity signals should also decrease. Equally, by reducing the amount of IL, the availability of binding sites is lessened; so the competition for one binding site between two analytes increases. Table 5 (top) lists the values obtained from the WRF analysis. Once again; they are the result of peak area integration and mass correction analysis of the response obtained (figure S10 (a)). In the first instance; the conductivity values are uniformly shifted down. This is to be expected; as the concentration ratio of the IL has been reduced. The selective downward trend based on the nature of metal ion co-ordination still remains. Both WRF and EIS still complement each other in that the inverse trend of increased impedance for the co-ordinated membranes is still evident. This can be seen by looking at figure 5 (left) and table 4 (top) which summarises the results. What can also be observed is that the impedance for all membranes is significantly increased due to the increased concentration of PVC. Once again a correlation analysis of the respective responses from both EIS and WRF was undertaken (Figure S7). Again both trends are linear and serve to complement both techniques. A summary of the XRF analysis can be seen in table 6 (top). XRF once again proves to be a valid tool to explain the EIS and WRF results obtained previously. The levels of both Cu and Co in the membrane serve to validate both the conductivity and impedance trends seen for both WRF and EIS respectively. Once again Cu levels prevail over Co in all cases, which again are a reflection of the co-ordinating chemistry of the ligand [DCA]-. What is interesting to note from both EIS and XRF analyses; is that the selectivity of the IL for Cu2+ over Co2+ has increased substantially when compared to the first case studied. This is most likely a combination of the decreased concentration of binding sites resulting in an increased competition between two analytes for one ligand plus also the fact that we have consistently observed a higher preference of the membranes for Cu2+ over Co2+. 4.4 Membrane Component Ratio 1:2, IL:PVC. By further increasing the concentration of PVC to 66wt%, the resulting membranes became more inflexibile and brittle. A further reduced IL content means they have become primarily hydrophobic, which will impede their ability to uptake and bind metal ions. This proved to be a hindrance for the WRF detection system; a summary of the results obtained can be viewed in table 5 (bottom) and figure S10 (b). Given that its response is based on the conductivity of a given sample, it proved capable of only detecting the blank membrane containing only 33w% IL. Any co-ordination that does occur within this particular set of membranes results in neutral co-ordinated networks; which will lower the conductivity even further. This had the result of lowering the conductivity outside the limitation of the WRF instrumental setup. This is a limitation of the current setup and will be the subject of future work. Again; the EIS spectra yielded no observable trend (Figure 5 (right) and table 4 (bottom)). The impedance for all membranes is again increased (approx. one order of magnitude) due to increasing the levels of PVC within the membrane. From the individual Bode plots -which depict the relationship between the modulus of impedance and the scanning frequency- the impedance shift for the blank membrane is linear for both IL and PVC concentrations, which can be seen in figures S8 and S9. The XRF analysis proved helpful to validate the previously unexpected EIS trend (Table 6 (bottom)). Here the highest concentration of metal in the membrane was found to be the mixture, which corresponds to the highest impedance response seen for these membranes. The next highest levels are seen for Cu, whilst Co levels proved undetectable which correlates perfectly with the EIS response trend. The EIS spectra obtained are therefore directly related to the level of ion transfer and co-ordination within the membrane. 5. Conclusion In this work we have demonstrated that our IL based membranes do act as electroactive materials which; when co-ordinated to heavy metals provide a measured sensor response. We have also effectively demonstrated the use of WRF technology for this purpose and shown how the results obtained from 3 differing techniques definitively summarise the inherent co-ordinating chemistry of these membranes. In this case the IL based polymeric optodes are capable of discriminatory co-ordination of the heavy metals Cu2+, Co2+ and both ions in a mixture which produces an equal discriminatory conductivity decrease in the WRF signal. By documenting the inverse trend of impedance, we have validated this novel conductivity result. Both the WRF and EIS trends were then easily explained by studying the level of ion transfer and the co-ordinating preferences of the IL ligand [DCA]-. This was achieved by quantifying the amount of metal present in the membrane using XRF. By examining the case of Cu2+ co-ordination; the three detection techniques can be summarised as follows: Cu2+ exhibits the highest binding preferentiality to the IL (XRF), thereby producing the lowest WRF signal and the highest EIS response. The opposite then applies for Co2+ co-ordination with the mixture inevitably in between. With this and our previous work, we have now effectively shown how incorporation of a ligand as part of an IL can dramatically simplify a polymeric based optodes composition, and how both the inherent optical and transduction processes can be monitored using a variety of detection techniques. As we have now gained a valid insight into the electrical effects of metal- ion co-ordination in polymeric membranes through variation of its constituents; future work will be aimed at optimising important analytical characteristics such as the effects of changing of the IL cation and optimising the effects of analyte concentration. As mentioned previously ILs have been shown to bind to a range of d-block elements, plus important target analytes such as CO2  ADDIN EN.CITE Bates2002525217Bates, E. D.Mayton, R. D.Ntai, I.Davis, J. H.CO2 capture by a task-specific ionic liquidJournal of the American Chemical SocietyJournal of the American Chemical Society926-92712462002Feb0002-7863ISI:000173783500020<Go to ISI>://000173783500020 [49], benzaldehyde and acetone  ADDIN EN.CITE Tseng242417Tseng, M. C.Chu, Y. H.Chemoselective gas sensing ionic liquidsChemical CommunicationsChemical Communications2983-298546171359-7345ISI:000276632800029<Go to ISI>://000276632800029 [50]. Recently they have been shown to act as direct sensing materials for acids in aqueous and non-aqueous environments ADDIN EN.CITE Zhang2011868617Zhang, QinghuaZhang, ShiguoLiu, ShiminMa, XiangyuanLu, LiujinDeng, YouquanIonic liquid-modified dyes and their sensing performance toward acids in aqueous and non-aqueous solutionsAnalystAnalyst1302-130413672011The Royal Society of Chemistryhttp://dx.doi.org/10.1039/C0AN00885K [51]. If a change in conductivity can be presumed upon binding to the analyte, then the inherent conductivity properties of ILs should also change. The use of wireless conductivity monitoring also has many potential advantages, such as remote, autonomous monitoring. By combining the many advantageous properties of both ILs and conductivity detection, then dramatic gains in sensing materials AND detection can be achieved. 6. Acknowledgements This work is supported by Science Foundation Ireland under grant 07/CE/I1147 including the SFI-funded National Access Programme (NAP) grant NAP210 and by Enterprise Ireland grant 07/RFP/MASF812, which is part of EU-MATERA initiative. AK and AR would like to thank Dr. Al Robertson from CYTEC Industries for the generous donation of the IL used in this work. 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The intergral is then corrected by each individual mass reading, and by subtracting the background value. Mass: (g)IstartIendImeanXstartXendXBlankIntegral (raw)Integral (mass corrected)Blank0.2309 1638.9 1611.6 1625.25 56953963384.75 75503.8 52486.14 Copper0.2221 1636.2 1632 1634.1 52913963729.9 72456.8 39292.66 Cobalt0.2317 1625.6 1629.4 1627.5 48894166727.5 76801.8 43479.93 Mix0.2277 1629.2 1633 1631.1 47894268506.2 77675.17 40267.75  Figure S2: WRF Peak area analysis for membranes containing IL:PVC, 2:1. electrode thicknesselectrode + membrane thicknessmembrane thicknessmmmmmm10.2410.344250.1117520.2320.348250.1157530.2330.332250.0997540.2340.329250.0967550.2450.335250.1027560.22560.344250.11175average0.232570.349250.11675stdev0.00612372480.367250.1347590.343750.11125average membrane thickness0.111stdev0.011  Figure S3: Electrode and membrane thickness analysis for membranes containing 33wt% PVC. electrode thicknesselectrode + membrane thicknessmmmm10.2410.596520.2320.621530.2330.542540.2340.561550.2450.535560.22560.5435average0.232570.5705stdev0.00612372480.540590.5395average0.561stdev0.0299average membrane thickness0.328  Figure S4: Electrode and membrane thickness analysis for membranes containing 50wt% PVC. electrode thicknesselectrode + membrane thicknessmmmm10.2410.6662520.2320.6482530.2330.6692540.2340.6252550.2450.5962560.22560.65825average0.232570.63925stdev0.00612372480.6452590.65325average0.644stdev0.022average membrane thickness0.412  Figure S5: Electrode and membrane thickness analysis for membranes containing 66wt% PVC.   Figure S6: Detailed analysis of response obtained for membranes containing 2:1 (IL : PVC). Here the parameters on the x-axes represent (for WRF) 1 = Copper; 2 = Mix and 3 = Cobalt. For EIS; 1 = Cobalt, 2= Mix and 3 = Copper.   Figure S7: Detailed analysis of response obtained for membranes containing 2:1 (IL : PVC). Here the parameters on the x-axes represent (for WRF) 1 = Copper; 2 = Mix and 3 = Cobalt. For EIS; 1 = Cobalt, 2= Mix and 3 = Copper.  Figure S8: Bode plots obtained for increasing IL concentrations  Figure S9: Top: Plot of Impedance versus IL concentration (left) and PVC concentration (right).  Mass: (g)IstartIendImeanXstartXendXBlank Integral (raw)Integral (mass corrected)Blank0.228416501650165052944269300 7293115879Copper0.224816651665166543874473260 748497068Cobalt0.22616561654165554964269510 7287914908Mixture0.2106166316651666.545874271552 735379428  Mass: (g)IstartIendImeanXstartXendXBlankIntegral (raw)Integral (mass corrected)Blank0.2261669.41670.5167034562240171.2 384357502Copper0.2325--------Mix0.233--------Cobalt0.2243-------- Figure S10: WRF response obtained for (a) membranes containing 1:1, IL: PVC and (b) 1:2, IL: PVC. Figures:  Figure 1: The WRF instrument used in this work. The sample to be analysed is placed in the insulating material (centre) and passed along the green carousel through the detection channel containing the transmitting and receiving electrodes.  Figure 2: The individual responses obtained from WRF for membranes with component ratio 2:1, IL: PVC. Here the RF signal (y-axis) is given in arbitrary units.  Figure 3: EIS spectra for membranes containing 2:1, IL:PVC; Here (i) is the blank (no metal ion exposure) run, whilst the coloured lines depict exposure to (ii) Cu2+ ions, (iii) a 1:1 (v/v) mixture of Cu2+ and Co2+ ions and (iv) Co2+ ions. Inset: Equivalent Randles circuit representation used to obtain experimental data; where RCT is the membrane resistance of charge transfer, Q is constant phase element and ZW is Warburg impedance. C 1nF is the capacitance bridge used between the working and reference electrodes.  Figure 4: XRF spectra obtained for membranes with component ratio 2:1, IL: PVC. Here the black peaks are (i) no metal ion exposure (blank), whilst the coloured peaks correlate to membranes exposed to (ii) Cu2+ ions, (iii) a 1:1 (v/v) mixture of Cu2+ and Co2+ ions and (iv) Co2+ ions.  Figure 5: EIS results obtained for membranes containing 1:1, IL: PVC (left), and membranes containing 2:1, IL: PVC (right). For both cases; (i) no metal ion exposure (blank), (ii) exposure to Cu2+ ions, (iii) a 1:1 (v/v) mixture of Cu2+ and Co2+ ions and (iv) Co2+ ions. Tables: Membrane Composition:Blank:Copper:Mix:Cobalt:2:1, IL: PVC52486392924026743479 Table 1: Summary of WRF results for membranes containing 2:1 (IL : PVC); the values quoted are the result of peak area integration and mass correction analysis. Membrane:RCT: (): (S/cm)Blank36943.346 x 10-5Cobalt151407.362 x 10-6Mix161807.64 x 10-6Copper167908.165 x 10-6 Table 2: Resistance of charge transfer and conductivity values obtained via EIS analysis for membranes with component ratio 2:1, IL: PVC. 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