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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. 

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.