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Abstract As one of the noninvasive screening and diagnostic tools for human breath monitoring of various diseases, chemiresistive devices with nanomaterials as the sensing interfaces for detecting volatile organic compounds (VOCs) have attracted increasing interests. A key challenge for the practical applications is an effective integration of all components in a system level. By integrating with the system components, it provides reliable and rapid results as a fast‐screening method for healthcare, safety, and environmental monitoring. This paper highlights some of the latest developments in chemiresistive sensors designed for the detection of VOCs and human breaths. It begins with a brief introduction to the fundamental principles of chemiresistive sensors with nanoparticle‐structured sensing interfaces. This is followed by a discussion of the recent fabrication methods, with an emphasis on nanostructured materials. Some of the recent examples will be highlighted in terms of recent innovative approaches to sensor applications and system integrations. Challenges and opportunities will also be discussed for the advancement and refinement of the chemiresistive sensor technologies in breath screening and monitoring of diseases.more » « less
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Understanding the catalytic oxidation of propane is important for developing catalysts not only for catalytic oxidation of hydrocarbons in emission systems but also for selective oxidation in the chemical processing industry. For palladium-based catalysts, little is known about the identification of the chemical or intermediate species involved in propane oxidation. We describe herein findings of an investigation of the catalytic oxidation of propane over supported palladium nanoalloys with different compositions of gold (Pd n Au 100−n ), focusing on probing the chemical or intermediate species on the catalysts in correlation with the bimetallic composition and the alloying phase structure. In addition to an enhanced catalytic activity, a strong dependence of the catalytic activity on the bimetallic composition was revealed, displaying an activity maximum at a Pd : Au ratio of 50 : 50 in terms of reaction temperature. This dependence is also reflected by its dependence on the thermochemical treatment conditions. While the activity for nanoalloys with n ∼ 50 showed little change after the thermochemical treatment under oxygen, the activities for nanoalloys with n < 50 and n > 50 showed opposite trends. Importantly, this catalytic synergy is linked to the subtle differences of chemical and intermediate species which have been identified for the catalysts with different bimetallic compositions by in situ measurements using diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). For the catalytic oxidation of propane over the highly-active catalyst with a Pd : Au ratio of 50 : 50, the major species identified include acetate and bicarbonate, showing subtle differences in comparison with the identification of bicarbonate and formate for the catalyst with <50% Au (with a lower activity) and the absence of apparent species for the catalyst with >50% Au (activity is largely absent). The alloying of 50% Au in Pd is believed to increase the oxophilicity of Pd, which facilitates the first carbon–carbon bond cleavage and oxygenation of propane. The implications of the findings on the catalytic synergy of Pd alloyed with Au and the design of active Pd alloy catalysts are also discussed.more » « less
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There has been an increasing need of technologies to manufacturing chemical and biological sensors for various applications ranging from environmental monitoring to human health monitoring. Currently, manufacturing of most chemical and biological sensors relies on a variety of standard microfabrication techniques, such as physical vapor deposition and photolithography, and materials such as metals and semiconductors. Though functional, they are hampered by high cost materials, rigid substrates, and limited surface area. Paper based sensors offer an intriguing alternative that is low cost, mechanically flexible, has the inherent ability to filter and separate analytes, and offers a high surface area, permeable framework advantageous to liquid and vapor sensing. However, a major drawback is that standard microfabrication techniques cannot be used in paper sensor fabrication. To fabricate sensors on paper, low temperature additive techniques must be used, which will require new manufacturing processes and advanced functional materials. In this work, we focus on using aerosol jet printing as a highresolution additive process for the deposition of ink materials to be used in paper-based sensors. This technique can use a wide variety of materials with different viscosities, including materials with high porosity and particles inherent to paper. One area of our efforts involves creating interdigitated microelectrodes on paper in a one-step process using commercially available silver nanoparticle and carbon black based conductive inks. Another area involves use of specialized filter papers as substrates, such as multi-layered fibrous membrane paper consisting of a poly(acrylonitrile) nanofibrous layer and a nonwoven poly(ethylene terephthalate) layer. The poly(acrylonitrile) nanofibrous layer are dense and smooth enough to allow for high resolution aerosol jet printing. With additively fabricated electrodes on the paper, molecularly-functionalized metal nanoparticles are deposited by molecularly-mediated assembling, drop casting, and printing (sensing and electrode materials), allowing full functionalization of the paper, and producing sensor devices with high surface area. These sensors, depending on the electrode configuration, are used for detection of chemical and biological species in vapor phase, such as water vapor and volatile organic compounds, making them applicable to human performance monitoring. These paper based sensors are shown to display an enhancement in sensitivity, as compared to control devices fabricated on non-porous polyimide substrates. These results have demonstrated the feasibility of paper-based printed devices towards manufacturing of a fully wearable, highly-sensitive, and wireless human performance monitor coupled to flexible electronics with the capability to communicate wirelessly to a smartphone or other electronics for data logging and analysis.more » « less
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Surface‐Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D SensorsAbstract Fibrous materials serve as an intriguing class of 3D materials to meet the growing demands for flexible, foldable, biocompatible, biodegradable, disposable, inexpensive, and wearable sensors and the rising desires for higher sensitivity, greater miniaturization, lower cost, and better wearability. The use of such materials for the creation of a fibrous sensor substrate that interfaces with a sensing film in 3D with the transducing electronics is however difficult by conventional photolithographic methods. Here, a highly effective pathway featuring surface‐mediated interconnection (SMI) of metal nanoclusters (NCs) and nanoparticles (NPs) in fibrous materials at ambient conditions is demonstrated for fabricating fibrous sensor substrates or platforms. Bimodally distributed gold–copper alloy NCs and NPs are used as a model system to demonstrate the semiconductive‐to‐metallic conductivity transition, quantized capacitive charging, and anisotropic conductivity characteristics. Upon coupling SMI of NCs/NPs as electrically conductive microelectrodes and surface‐mediated assembly (SMA) of the NCs/NPs as chemically sensitive interfaces, the resulting fibrous chemiresistors function as sensitive and selective sensors for gaseous and vaporous analytes. This new SMI–SMA strategy has significant implications for manufacturing high‐performance fibrous platforms to meet the growing demands of the advanced multifunctional sensors and biosensors.more » « less
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