Introducing Molecular Functionalities within High Surface Area Nanostructured ITO Electrodes through Diazonium Electrografting

Kim, Yee-Seul; Fournier, Sophie; Lau-Truong, Stéphanie; Decorse, Philippe; Devillers, Charles H.; Lucas, Dominique; Harris, Kenneth D. M.; Limoges, Benoı̂t; Balland, Véronique

doi:10.1002/celc.201800418

Cited by 15 publications

(15 citation statements)

References 39 publications

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“…For example, mixed monolayers made of organophosphonic derivatives have been electrografted onto nitinol (NiTi), which is an alloy often employed in the biomedical field, in order to prevent the release of the possibly carcinogenic Ni 2+ ions [327]. Kim et al [143] modified a GLAD-ITO substrate by the electrografting of a porphyrin diazonium salt, showing the possibility to introduce molecular functionalities, such as photo-activity Numerous examples can be found in the literature reporting molecular electronic devices based on the electrografting of diazonium salts. Here, it is noteworthy the pioneering work done in the group of McCreery [321,322], that reported the first all-carbon based molecular tunnel junctions.…”

Section: The Electrografting Techniquementioning

confidence: 99%

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

2020

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The societal impact of the electronics industry is enormous—not to mention how this industry impinges on the global economy. The foreseen limits of the current technology—technical, economic, and sustainability issues—open the door to the search for successor technologies. In this context, molecular electronics has emerged as a promising candidate that, at least in the short-term, will not likely replace our silicon-based electronics, but improve its performance through a nascent hybrid technology. Such technology will take advantage of both the small dimensions of the molecules and new functionalities resulting from the quantum effects that govern the properties at the molecular scale. An optimization of interface engineering and integration of molecules to form densely integrated individually addressable arrays of molecules are two crucial aspects in the molecular electronics field. These challenges should be met to establish the bridge between organic functional materials and hard electronics required for the incorporation of such hybrid technology in the market. In this review, the most advanced methods for fabricating large-area molecular electronic devices are presented, highlighting their advantages and limitations. Special emphasis is focused on bottom-up methodologies for the fabrication of well-ordered and tightly-packed monolayers onto the bottom electrode, followed by a description of the top-contact deposition methods so far used.

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Section: The Electrografting Techniquementioning

confidence: 99%

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

2020

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“…They also confirm that the diazoniumelectrografting strategy is a viable approach to functionalizing ITO surfaces with stable and highly robust molecular layers. [11][12][13] It should be noted, however, that the   value is strongly dependent on the nature of the immobilized molecule. In the case of Fc-NHCO,   is equivalent to ~13 saturated monolayers of Fc-NH 2 on a planar electrode, which, once compared to the ~65 surface enhancement of the 1 m-thick nanostructured GLAD-ITO film, leads to the conclusion that only 20% of a saturated monolayer is covering the three-dimensional surface.…”

Section: Electrochemical Characterization Of Amidoferrocenementioning

confidence: 99%

“…A better alternative, which has recently emerged in the literature for the surface-functionalization of meso-TCEs, is to take advantage of the covalent electrochemical grafting of aryl-diazonium salts. [11][12][13] This method is highly versatile, simple, efficient and able to operate with a wide range of metal oxide surfaces. Also, because this is an electrodeposition approach, it offers the additional advantage of reliably grafting molecules on conductive surfaces, regardless of their shapes and porosities.…”

Section: Introductionmentioning

confidence: 99%

“…The method was successfully applied to the robust surface modification of meso-TCE electrodes with redox active dyes, leading to improved stability under hydrolytic aqueous conditions as compared to other surface functionalization chemistries. [11][12][13] Herein, we prepare robust GLAD-ITO electrodes pre-functionalized with carboxylate moieties through the electrochemical reduction of aryl diazonium salts. The resulting pre-functionalized electrodes are then used as a versatile platform for further covalent immobilization of the bioreceptor hemoglobin I from Lucina pectinata.…”

Section: Introductionmentioning

confidence: 99%

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An optical H2S biosensor based on the chemoselective Hb-I protein tethered to a transparent, high surface area nanocolumnar electrode

Dulac

Melet

Harris

et al. 2019

Sensors and Actuators B: Chemical

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Sensitive and selective detection of analytes in complex biological fluids can be an extremely challenging issue. The constructive association of biomolecules and transparent mesoporous electrodes is of interest in this area, as it can lead to innovative biosensors combining optical and electrochemical detection modes. This concept, however, requires the development of appropriate surface functionalization methodologies that are robust enough for long-term operation in physiological environments. In the present work, the high-surface area of 3D transparent mesoporous indium-tin oxide (ITO) electrodes (prepared by glancing angle deposition or GLAD) has been chemically functionalized with recombinant hemoglobin I from Lucina pectinata according to a versatile 2-step process. First, 4-diazoniumbenzoic acid salt is covalently electrografted onto the ITO surface, followed by amide coupling of the protein. The resulting electrodes were quantitatively characterized by cyclic voltammetry and UV-visible absorption spectroscopy, demonstrating high surface coverages (up to 45% of a closed-packed monolayer for Hemoglobin-I) and homogeneous distribution across the entire thickness of the GLAD mesoporous structure. Good stability is also observed when the modified electrodes are immersed for prolonged times in a high ionic strength saline buffer. We also show that the hemoglobin I-modified electrode can be used as an optical biosensor for the selective, reversible, and fast detection of H 2 S in aqueous solutions over a two-decade concentration range and with a limit of detection of 0.35 M. Good analytical performance was also achieved in human plasma without significant interference from the biological matrix.

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“…These applications require the preparation of thin films of porphyrin/metalloporphyrin derivatives on solid substrates. For this purpose, they should be deposited onto a substrate by various coating techniques such as Langmuir‐Blodgett , self‐assembly , spin coating , electropolymerization or diazonium salt modification method . Among them, the modification of a substrate surface via electrochemical/chemical reduction of diazonium salts is a simple and effective procedure for the preparation of organic films on surfaces since robust organic films with controlled thickness can be determined by this method .…”

Section: Introductionmentioning

confidence: 99%

Electrocatalytic Reduction of Oxygen at Glassy Carbon Electrodes Coated with Diazonium‐derived Porphyrin/Metalloporphyrin Films

et al. 2020

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In this study, the influence of the film structure was investigated on the electrocatalytic oxygen reduction at GC electrodes covered with porphyrin and metalloporphyrin rings via the diazonium modification method. For that purpose, primarily, tetraphenylporphyrin (TPP) films on GC electrode surfaces were prepared by electroreduction of in situ generated diazonium salts of 5‐(4‐aminophenyl)‐10,15,20‐triphenylporphyrin (APP) and 5,10,15,20‐tetrakis(4‐aminophenyl)porphyrin (TAPP) molecules. Next, the formation of metalloporphyrin films on the modified surfaces was accomplished through the complexation reactions of surface porphyrin rings with metal ions in the salt solutions containing Mn(II), Fe(III) and Co(II) ions. The resulting porphyrin and metalloporphyrin layers were identified with XPS and ICP‐MS. The electrochemical barrier properties of the films on GC surfaces were examined by cyclic voltammetry in K3Fe(CN)6 aqueous solution. The electrocatalytic abilities of the resulting films were also investigated for the oxygen electrochemical reduction by employing cyclic voltammetry in PBS solutions saturated with oxygen. The results showed that the oxygen reduction potentials on modified GC electrodes were shifted to less negative potentials compared to that of bare GC electrode. Also, it was obtained that the oxygen reduction reaction was more effective on the GC electrodes modified with TPP rings by using TAPP molecules than those prepared by using APP molecules.

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Introducing Molecular Functionalities within High Surface Area Nanostructured ITO Electrodes through Diazonium Electrografting

Cited by 15 publications

References 39 publications

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

Nanofabrication Techniques in Large-Area Molecular Electronic Devices

An optical H2S biosensor based on the chemoselective Hb-I protein tethered to a transparent, high surface area nanocolumnar electrode

Electrocatalytic Reduction of Oxygen at Glassy Carbon Electrodes Coated with Diazonium‐derived Porphyrin/Metalloporphyrin Films

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