We report on the synthesis of two new threaded BODIPYs 5 and 6 in good yields using boron as a gathering atom and a macrocycle with a 2,2'-biphenol unit. In addition to usual techniques, they were characterized by X-ray crystallography. Their electrochemical and optical properties were investigated.
View Article and Find Full Text PDFCu(I)-catalyzed 1,3-dipolar cycloaddition (CuAAC), also known as click chemistry, has been demonstrated to be highly robust while providing versatile surface chemistry. One specific application is biosensor fabrication. Recently, we developed thermoplastic electrodes (TPEs) as an alternative to traditional carbon composite electrodes in terms of cost, performance, and robustness.
View Article and Find Full Text PDFAs a semimetal with a zero band gap and single-atom-scale thickness, single layer graphene (SLG) has excellent electron conductivity on its basal plane. If the band gap could be opened and regulated controllably, SLG would behave as a semiconductor. That means electronic elements or even electronic circuits with single-atom thickness could be expected to be printed on a wafer-scale SLG substrate, which would bring about a revolution in Moore's law of integrated circuits, not by decreasing the feature size of line width, but by piling up the atomic-scale-thickness of an SLG circuit board layer by layer.
View Article and Find Full Text PDFIntroduction Advanced airway management by paramedics is potentially life-saving, but carries a significant risk to patient safety and can be associated with poor clinical outcome if performed incorrectly. Previously, our team had found that an intensive education intervention demonstrated an improvement in paramedic performance on a written exam and increased confidence in airway skills. This study measured intubation success and the number of attempts per patient before and after intensive paramedic airway management education intervention.
View Article and Find Full Text PDFSensitive and selective detection of biomarkers in serum in a short time has a significant impact on health. The enormous clinical importance of developing reliable methods and devices for testing serum levels of cardiac troponin I (cTnI), which are directly correlated to acute myocardial infarction (AMI), has spurred an unmatched race among researchers for the development of highly sensitive and cost-effective sensing formats to be able to differentiate patients with early onset of cardiac injury from healthy individuals with a mean cTnI level of 26 pg mL. Electronic- and electrochemical-based detection schemes allow for fast and quantitative detection not otherwise possible at the point of care.
View Article and Find Full Text PDFThe controlled covalent functionalization of the graphene channel of a field effect transistor, based on interdigitated gold electrodes (source and drain), electrochemical grafting, using specifically designed aryl diazonium species is demonstrated to allow the simple fabrication of a general platform for (bio)sensing applications. The electrochemical grafting of a protected ethynylphenyl diazonium salt leads to the deposition of only a monolayer on the graphene channel. This controlled covalent functionalization of the graphene channel results in a charge mobility of the GFET of 1739 ± 376 cm V s and 1698 ± 536 cm V s for the holes and electrons, respectively, allowing their utilization as (bio)sensors.
View Article and Find Full Text PDFThermoplastic electrodes (TPEs) are carbon composite electrodes consisting of graphite and thermoplastic polymer binder. TPE production is a solvent-based method, which makes it easy to fabricate and pattern into complex geometries, contrary to classical carbon composite electrodes. Depending on the composition (carbon type, binder, and composition ratio), TPEs can give excellent electrochemical performance and high conductivity.
View Article and Find Full Text PDFThe incorporation of terminal alkynes into the chemical structure of persistent organic perchlorotriphenylmethyl (PTM) radicals provides new chemical tools to expand their potential applications. In this work, this is demonstrated by the chemical functionalization of two types of substrates, hydrogenated SiO-free silicon (Si-H) and gold, and, by exploiting the click chemistry, scarcely used with organic radicals, to synthesise multifunctional systems. On one hand, the one-step functionalization of Si-H allows a light-triggered capacitance switch to be successfully achieved under electrochemical conditions.
View Article and Find Full Text PDFIntroduction: Certain adult conditions treated by paramedics, such as myocardial infarction or stroke, have better outcomes if transported to a specialty centre, bypassing local generalist facilities when necessary. Little evidence exists to inform guidelines to identify pediatric patients who would benefit from direct transport to a pediatric centre. This study describes the characteristics of children brought to community emergency departments (ED) who subsequently required transfer to pediatric specialty care.
View Article and Find Full Text PDFFor the purpose of preparing well-organized functional surfaces, carbon and gold substrates were modified using electroreduction of a tetrahedral-shape preorganized tetra-aryldiazonium salt, leading to the deposition of ultrathin organic films. Characterization of the modified surfaces has been performed using cyclic voltammetry, X-ray photoelectron spectroscopy, infrared absorption spectroscopy, ellipsometry, atomic force microscopy, and contact angle measurements. The specific design of the tetra-aryldiazonium salts leads to an intrinsic structuring of the resulting organic films, allowing molecular sieving and current rectification properties toward redox probes in solution.
View Article and Find Full Text PDFWhilst most studies in single-molecule electronics involve components first synthesized , there is also great potential in exploiting chemical transformations to prepare devices . Here, as a first step towards this goal, we conduct reversible reactions on monolayers to make and break covalent bonds between alkanes of different lengths, then measure the conductance of these molecules connected between electrodes using the scanning tunneling microscopy-based break junction (STM-BJ) method. In doing so, we develop the critical methodology required for assembling and disassembling surface-bound single-molecule circuits.
View Article and Find Full Text PDFThe reactivity of functionalized ynamides and arylynamines with tetracyanoethylene at room temperature was evaluated. In most cases, the corresponding 1,1,4,4-tetracyanobutadienes (TCBDs) were obtained in good to excellent yields through a [2+2]-cycloaddition/[2+2]-retro-electrocyclization sequence. The influence of diverse functional groups on the yield of the reaction was investigated, in particular concerning multiple ynamides.
View Article and Find Full Text PDFScanning electrochemical microscopy (SECM) is used for studying the intrinsic photo-electrochemical properties of CdSe/CdS quantum rods. They are deposited on a transparent and non-conductive glass plate and investigated by SECM in feedback and generator-collector modes using a series of redox mediators. The method allows the interrogation of the quantum rods under illumination without the interference of the substrate, notably that due to the electron photo-ejection from the substrate, a process that is inherent to any polarized electrode material.
View Article and Find Full Text PDFBackground: Few studies have established that obesity promotes all types of urinary incontinence and disorders of the pelvic floor. The role of bariatric surgery in urinary incontinence remains poorly studied.
Objective: To determine the effect of bariatric surgery on urinary incontinence, dysuria, and fecal incontinence before and 1 year after bariatric surgery.
J Am Chem Soc
October 2016
The immobilization of a copper calix[6]azacryptand funnel complex on gold-modified electrodes is reported. Two different methodologies are described. One is based on alkyne-terminated thiol self-assembled monolayers.
View Article and Find Full Text PDFGold nanoparticles stabilized with a thin layer of post-functionalizable calix[4]arenes were prepared through the reductive grafting of a calix[4]arene-tetra-diazonium salt. These particles show exceptional stability towards extreme pH, F(-), NaCl, and upon drying. Post-functionalization of the calix-layer was demonstrated, opening the way to a wide range of applications.
View Article and Find Full Text PDFAminophenyl and aminomethylphenyl monolayers have been electrografted to glassy carbon and pyrolyzed photoresist film from the corresponding diazonium ions using a protection-deprotection strategy based on Boc (tert-butyloxycarbonyl) and Fmoc (fluorenylmethyloxycarbonyl) groups. After grafting and then deprotecting films of Boc-NH-Ar, Fmoc-NH-Ar, and Fmoc-NH-CH2-Ar, depth profiling by atomic force microscopy confirmed that the resulting amine-terminated films were monolayers. In contrast, after deprotection, Boc-NH-CH2-Ar gave a multilayer film.
View Article and Find Full Text PDFCharge transport through an insulating layer was probed using ferrocenyl-terminated dendrimers and scanning electrochemical microscopy. Experiments show that the passage through the layer is considerably enhanced when the transferred charges are brought globally to the surface by the ferrocenyl dendrimer instead of a single ferrocene molecule. This result shows that charge tunneling through an insulator could be promoted by a purely molecular nano-object.
View Article and Find Full Text PDFA high-yielding sequence of [2+2] cycloaddition-retroelectrocyclization of ynamides with tetracyanoethylene (TCNE) is described. The reaction provided tetracyanobutadiene (TCBD) species, which were characterized by various techniques. DFT and TD-DFT calculations were also performed to complement experimental findings.
View Article and Find Full Text PDFElectrografting of aryl films to electrode surfaces from diazonium ion solutions is a widely used method for preparation of modified electrodes. In the absence of deliberate measures to limit film growth, the usual film structure is a loosely packed multilayer. For some applications, monolayer films are advantageous; our interest is in preparing well-defined monolayers of reactive tethers for further on-surface chemistry.
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