Acetone in the human breath is an important marker for noninvasive diagnosis of diabetes. Here, novel chemo-resistive detectors have been developed that allow rapid measurement of ultralow acetone concentrations (down to 20 ppb) with high signal-to-noise ratio in ideal (dry air) and realistic (up to 90% RH) conditions. The detector films consist of (highly sensitive) pure and Si-doped WO(3) nanoparticles (10-13 nm in diameter) made in the gas phase and directly deposited onto interdigitated electrodes. Their sensing properties (selectivity, limit of detection, response, and recovery times) have been investigated as a function of operating temperature (325-500 degrees C), relative humidity (RH), and interfering analyte (ethanol or water vapor) concentration. It was found that Si-doping increases and stabilizes the acetone-selective epsilon-WO(3) phase while increasing its thermal stability and, thus, results in superior sensing performance with an optimum at about 10 mol % Si content. Furthermore, increasing the operation temperature decreased the detector response to water vapor, and above 400 degrees C, it was (or=1800 ppb) can be clearly distinguished by a remarkable gap (40%) in sensor response. As a result, these solid state detectors may offer a portable and cost-effective alternative to more bulky systems for noninvasive diabetes detection by human breath analysis.

Since the development of the first chemoresistive metal oxide based gas sensors, transducers with innovative properties have been prepared by a variety of wet- and dry-deposition methods. Among these, direct assembly of nanostructured films from the gas phase promises simple fabrication and control and with the appropriate synthesis and deposition methods nm to μm thick films, can be prepared. Dense structures are achieved by tuning chemical or vapor deposition methods whereas particulate films are obtained by deposition of airborne, mono- or polydisperse, aggregated or agglomerated nanoparticles. Innovative materials in non-equilibrium or sub-stoichiometric states are captured by rapid cooling during their synthesis. This Review presents some of the most common chemical and vapor-deposition methods for the synthesis of semiconductor metal oxide based detectors for chemical gas sensors. In addition, the synthesis of highly porous films by novel aerosol methods is discussed. A direct comparison of structural and chemical properties with sensing performance is given.

Breath analysis has the potential for early stage detection and monitoring of illnesses to drastically reduce the corresponding medical diagnostic costs and improve the quality of life of patients suffering from chronic illnesses. In particular, the detection of acetone in the human breath is promising for non-invasive diagnosis and painless monitoring of diabetes (no finger pricking). Here, a portable acetone sensor consisting of flame-deposited and in situ annealed, Si-doped epsilon-WO 3 nanostructured films was developed. The chamber volume was miniaturized while reaction-limited and transport-limited gas flow rates were identified and sensing temperatures were optimized resulting in a low detection limit of acetone (~20 ppb) with short response (10-15 s) and recovery times (35-70 s). Furthermore, the sensor signal (response) was robust against variations of the exhaled breath flow rate facilitating application of these sensors at realistic relative humidities (80-90%) as in the human breath. The acetone content in the breath of test persons was monitored continuously and compared to that of state-of-the-art proton transfer reaction mass spectrometry (PTR-MS). Such portable devices can accurately track breath acetone concentration to become an alternative to more elaborate breath analysis techniques.

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Formaldehyde (FA) is a potential breath marker for lung cancer and a tracer for indoor air quality monitoring. Its typical concentrations are below 100 ppb posing a sensitivity and selectivity challenge to current portable sensor systems. Here, we present a highly sensitive, selective, and compact electronic nose (E-nose) for real-time quantification of FA at realistic conditions. This E-nose consists of four nanostructured and highly porous Pt-, Si-, Pd-, and Tidoped SnO 2 sensing films directly deposited onto silicon wafer-based microsubstrates by flame spray pyrolysis (FSP). The constituent sensors offer stable responses (24 h tested) and detection of FA down to 3 ppb (signal-to-noise ratio > 25) at breath-realistic 90% relative humidity. Each dopant induces different analyte selectivity enabling selective detection of FA in two-, three-and four-analyte mixtures by multivariate linear regression. In simulated breath (FA with higher acetone, NH 3 , and ethanol concentrations), FA is detected with an average error ≤ 9 ppb using the present E-nose and overcoming selectivity issues of single sensors. This device could facilitate easy screening of lung cancer patients and monitoring of indoor FA concentrations.

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Acetone in the human breath is a key marker for noninvasive diagnosis of diabetes. Here, sensing films of pure and SiO2-doped WO3 nanoparticles have been made, directly deposited and in situ annealed onto interdigitated electrodes by scalable flame aerosol technology. A unique innovation here is that these films consist of ε-WO3, a metastable phase that has a high selectivity to acetone. The effect of nontoxic Si doping on the ε-phase content and crystal and grain sizes was investigated and correlated to the acetone sensing performance of these films. The thermal stability of these materials was characterized as well, revealing a unique opportunity for reliable sensing of acetone and noninvasive diagnostics of diabetes. An optimal doping level with 10 mol % SiO2 resulted in highly sensitive and highly selective acetone sensors down to 20 ppb.

Transparent, pure SiO(2), TiO(2), and mixed silica-titania films were (stochastically) deposited directly onto glass substrates by flame spray pyrolysis of organometallic solutions (hexamethyldisiloxane or tetraethyl orthosilicate and/or titanium tetra isopropoxide in xylene) and stabilized by in situ flame annealing. Silicon dioxide films consisted of a network of interwoven nanofibers or nanowires several hundred nm long and 10-15 nm thick, as determined by microscopy. These nanowire or nanofibrous films were formed by chemical vapor deposition (surface growth) on bare glass substrates during scalable combustion of precursor solutions at ambient conditions, for the first time to our knowledge, as determined by thermophoretic sampling of the flame aerosol and microscopy. In contrast, titanium dioxide films consisted of nanoparticles 3-5 nm in diameter that were formed in the flame and deposited onto the glass substrate, resulting in highly porous, lace-like nanostructures. Mixed SiO(2)-TiO(2) films (40 mol % SiO(2)) had similar morphology to pure TiO(2) films. Under normal solar radiation, all such films having a minimal thickness of about 300 nm completely prevented fogging of the glass substrates. These anti-fogging properties were attributed to inhibition of water droplet formation by such super-hydrophilic coatings as determined by wetting angle measurements. Deactivated (without UV radiation) pure TiO(2) coatings lost their super-hydrophilicity and anti-fogging properties even though their wetting angle was reduced by their nanowicking. In contrast, SiO(2)-TiO(2) coatings exhibited the best anti-fogging performance at all conditions taking advantage of the high surface coverage by TiO(2) nanoparticles and the super-hydrophilic properties of SiO(2) on their surface.