Advanced Composite for sp3‐Carbon‐Based Gas Sensing Application from Gold Organometallic Single Nanolayering on Diamondoids
Source abstract
Abstract
Abstract The assembly of hybrid materials combining a pure sp3‐C platform from nano‐and microcrystals of molecularly‐defined nanometer‐sized functionalized diamondoids (nanodiamonds) coated with a gold transition metal nanolayer is conducted from the gas phase, following a two‐steps vapor phase dry construction process. By using first the controlled vapor phase self‐assembly of primary phosphine diamantane derivatives, followed by a chemical vapor decomposition of a suited gold organometallic complex the synthesis of the nanocomposite Au@H2P–DiamOH 2 is achieved. The gold deposit surface analysis reveals the formation of a Au–P covalent bonding, which excludes the formation of phosphine oxide, as confirmed at higher depth into the nanocomposite by Hard X‐ray Photoelectron Spectroscopy analysis (HaXPES). The thickness d of the gold layers deposited onto the surface of diamondoids is estimated to be around d = 0.8 ± 10% nm from XPS data, which allows combining the composite Au@H2P–DiamOH 2 with ITO interdigitated electrodes, to produce a long‐life, highly stable and reproducible, n‐type behavior sensor for ammonia detection. A relative response (RR) of 150% at 30 ppm and a limit of detection of 6 ppm are measured at room temperature (20 to 25 °C) and at 45% of relative humidity.
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Research context
OpenAlex topics: Molecular Junctions and Nanostructures · Diamond and Carbon-based Materials Research · Advanced Memory and Neural Computing
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Institut de Chimie Moléculaire de l'Université de Bourgogne (ICMUB), UMR CNRS 6302 Université de Bourgogne 9 avenue Alain Savary Dijon 21078 France
Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB), UMR CNRS 6303 Université de Bourgogne 9 avenue Alain Savary Dijon 21078 France
Funding
Centre National de la Recherche Scientifique · Université de Bourgogne · European Regional Development Fund · Conseil régional de Bourgogne-Franche-Comté
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70. The photoemission signals C1s and Auger C KLL correspond to very different kinetic energies of ca. 1200 eV and 240 eV respectively. Their attenuation through the gold film is different and can be expressed asI=I0e−d/λ where I is the intensity of the detected signal I0is the intensity of the signal emitted by the diamondoid deposit when it is not covered by gold and λ is the inelastic mean free path (IMFP) of the electrons emitted through gold. For each energy i.e. for each signal λ can be easily determined using the TPP‐2 M model (Tanuma‐Powell‐Penn seeSurf. Interface Anal.1997 25 25). Intensity ratio rather than direct intensities are used. The intensities of the signals detected for the core level C1s and for the Auger signal CKLL are written respectively:IC1s=I0C1se−d/λC1s${I}\rm C1s = I_0\rm C1s{e}^{ - d/{\lambda }\rm C1s}$andICKLL=I0CKLLe−d/λCKLL${I}\rm CKLL = I_0\rm CKLL{e}^{ - d/\lambda {\rm CKLL}}$(IC1sandICKLLare the intensity of the detected signals C1s and CKLL respectively) I0C1s$I_0\rm C1s$andI0CKLL$I_0\rm CKLL$are the intensity of the signals C1s and CKLL from the native diamondoid deposit and λC1s and λCKLLare the inelastic mean free path (IMFP) of the electrons which constitute the signals C1s and CKLL through gold film. The ratio are expressed asIC1sICKLL=I0C1sI0CKLL×e−d/λC1se−d/λCKLL$\frac{{{I}\rm C1s}}{{{I}\rm CKLL}} = \frac{{I_0\rm C1s}}{{I_0\rm CKLL}} \times \frac{{{e}^{ - d/{\lambda }\rm C1s}}}{{{e}^{ - d/{\lambda }\rm CKLL}}}$andIC1sICKLL=I0C1sI0CKLL×e(λCKLL−λC1s)/d$\frac{{{I}C1s}}{{{I}\rm CKLL}} = \frac{{I_0\rm C1s}}{{I_0\rm CKLL}} \times e^{( {{\lambda }\rm CKLL - {\lambda }\rm C1s})/d}$from which the thicknessdcan be extracted. The determination of the ratio of the intensities of the signals C1s and CKLL is measured for a given coated sample and the same intensity ratio for a sample without gold deposit. Extraction of the thickness d can be achieved from O1s and OKLL signals following the same principle. The difference in energy between the O1s and OKLL signals being less important than between C1s and CKLL the result obtained may be less precise.
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72. From a mechanistic viewpoint charges need to flow across the resistive material as depicted inFigure7 for joinning the gold layer. Electrons provided by an incorporated DC voltage supply and connected to one of interdigitated electrode pass through the 10 µm thickness of the sensitive material (diamondoid scaffolding) in order to reach the less resistive gold monolayer and finish its path at the second interdigitated electrode by recrossing the resistive and sensitive material. This energy shortcut prevents the electrons from traveling a lateral interelectrode distance of ca. 75 µm in a mainly resistive diamondoid material and nicley explains the enhancement of the measured electric current using the gold composite.
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