Portable and inexpensive gas sensors are essential for the next generation of non-invasive medical diagnostics, smart air quality monitoring & control, human search & rescue and food quality assessment to name a few of their immediate applications. Therein, analyte selectivity in complex gas mixtures like breath or indoor air remains the major challenge. Filters are an effective and versatile, though often unrecognized, route to overcome selectivity issues by exploiting additional properties of target analytes (e.g., molecular size and surface affinity) besides reactivity with the sensing material. This review provides a tutorial for the material engineering of sorption, size-selective and catalytic filters. Of specific interest are high surface area sorbents (e.g., activated carbon, silica gels and porous polymers) with tunable properties, microporous materials (e.g., zeolites and metal–organic frameworks) and heterogeneous catalysts, respectively. Emphasis is placed on material design for targeted gas separation, portable device integration and performance. Finally, research frontiers and opportunities for low-cost gas sensing systems in emerging applications are highlighted.
Acetone is a toxic air pollutant and a key breath marker for non‐invasively monitoring fat metabolism. Its routine detection in realistic gas mixtures (i.e., human breath and indoor air), however, is challenging, as low‐cost acetone sensors suffer from insufficient selectivity. Here, a compact detector for acetone sensing is introduced, having unprecedented selectivity (>250) over the most challenging interferants (e.g., alcohols, aldehydes, aromatics, isoprene, ammonia, H2, and CO). That way, acetone is quantified with fast response (<1 min) down to, at least, 50 parts per billion (ppb) in gas mixtures with such interferants having up to two orders of magnitude higher concentration than acetone at realistic relative humidities (RH = 30–90%). The detector consists of a catalytic packed bed (30 mg) of flame‐made Al2O3 nanoparticles (120 m2 g−1) decorated with Pt nanoclusters (average size 9 nm) and a highly sensitive chemo‐resistive sensor made by flame aerosol deposition and in situ annealing of nanostructured Si‐doped ε‐WO3 (Si/WO3). Most importantly, the catalytic packed bed converts interferants continuously enabling highly selective acetone sensing even in the exhaled breath of a volunteer. The detector exhibits stable performance over, at least, 145 days at 90% RH, as validated by mass spectrometry.
More than 1 million workers are exposed routinely to carcinogenic benzene, contained in various consumer products (e.g., gasoline, rubbers, and dyes) and released from combustion of organics (e.g., tobacco). Despite strict limits (e.g., 50 parts per billion (ppb) in the European Union), routine monitoring of benzene is rarely done since low‐cost sensors lack accuracy. This work presents a compact, battery‐driven device that detects benzene in gas mixtures with unprecedented selectivity (>200) over inorganics, ketones, aldehydes, alcohols, and even challenging toluene and xylene. This can be attributed to strong Lewis acid sites on a packed bed of catalytic WO3 nanoparticles that prescreen a chemoresistive Pd/SnO2 sensor. That way, benzene is detected down to 13 ppb with superior robustness to relative humidity (RH, 10–80%), fulfilling the strictest legal limits. As proof of concept, benzene is quantified in indoor air in good agreement (R2 ≥ 0.94) with mass spectrometry. This device is readily applicable for personal exposure assessment and can assist the implementation of low‐emission zones for sustainable environments.
Mobile health technologies can provide information routinely and on demand to manage metabolic diseases (e.g., diabetes and obesity) and optimize their treatment (e.g., exercise or dieting). Most promising is breath acetone monitoring to track lipolysis and complement standard glucose monitoring. Yet, accurate quantification of acetone down to parts‐per‐billion (ppb) is difficult with compact and mobile devices in the presence of interferants at comparable or higher concentrations. Herein, a low‐cost detector that quantifies end‐tidal acetone during exercise and rest is presented with excellent bias (25 ppb) and unprecedented precision (169 ppb) in 146 breath samples. It combines a flame‐made Pt/Al2O3 catalyst with a chemoresistive Si/WO3 sensor. The detector is robust against orders of magnitude higher ethanol concentrations from disinfection and exercise‐driven endogenous breath isoprene ones, as validated by mass spectrometry. This detector accurately tracks the individual lipolysis dynamics in all volunteers, as confirmed by blood ketone measurements. It can be integrated readily into handheld devices for personalized metabolic assessment at home, in gyms, and clinics.
Exhaled breath acetone (BrAce) was investigated during and after submaximal aerobic exercise as a volatile biomarker for metabolic responsiveness in high and lower-fit individuals in a prospective cohort pilot-study. Twenty healthy adults (19–39 years) with different levels of cardiorespiratory fitness (VO 2peak ), determined by spiroergometry, were recruited. BrAce was repeatedly measured by proton-transfer-reaction time-of-flight mass spectrometry (PTR-TOF-MS) during 40–55 min submaximal cycling exercise and a post-exercise period of 180 min. Activity of ketone and fat metabolism during and after exercise were assessed by indirect calorimetric calculation of fat oxidation rate and by measurement of venous β-hydroxybutyrate (βHB). Maximum BrAce ratios were significantly higher during exercise in the high-fit individuals compared to the lower-fit group (t-test; p = 0.03). Multivariate regression showed 0.4% (95%-CI = −0.2%–0.9%, p = 0.155) higher BrAce change during exercise for every ml kg −1 min −1 higher VO 2peak . Differences of BrAce ratios during exercise were similar to fat oxidation rate changes, but without association to respiratory minute volume. Furthermore, the high-fit group showed higher maximum BrAce increase rates (46% h −1 ) in the late post-exercise phase compared to the lower-fit group (29% h −1 ). As a result, high-fit young, healthy individuals have a higher increase in BrAce concentrations related to submaximal exercise than lower-fit subjects, indicating a stronger exercise-related activation of fat metabolism.
Low‐cost metal oxide sensors are highly attractive for emerging applications such as breath analysis. Particularly promising are p‐type sensors that can operate at low temperatures, a key requirement for compact and low‐power devices. To date, however, these sensors lack sufficient sensitivity, selectivity, and humidity robustness to fulfil stringent requirements faced in real applications. Herein, a flame‐made and low‐power sensor (operated at 150 °C) that consists of CeO2‐decorated CuO nanoparticles is introduced, as determined by X‐ray diffraction and X‐ray photoelectron spectroscopy analysis. Most remarkably, this sensor features excellent robustness to 10–90% relative humidity. This is attributed to the presence of CeO2 nanoclusters, which may act by scavenging OH− and allow the readsorption of oxygen onto the CuO surface. To demonstrate its immediate impact, this sensor is investigated for the detection of acetone, a biomarker for fat burning. It detects acetone with high sensitivity (i.e., 50 ppb) and features excellent acetone selectivity (>9.8) toward key inorganic interferants (i.e., NH3, H2, and CO). Most importantly, the CeO2–CuO sensor accurately quantifies acetone concentrations in the exhaled breath of 16 volunteers (bias and precision of 90 and 457 ppb). As a result, it is attractive for low‐power and humidity robust detection of volatiles in breath analysis.