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Humans rely increasingly on sensors to address grand challenges and to improve quality of life in the era of digitalization and big data. For ubiquitous sensing, flexible sensors are developed to overcome the limitations of conventional rigid counterparts. Despite rapid advancement in bench-side research over the last decade, the market adoption of flexible sensors remains limited. To ease and to expedite their deployment, here, we identify bottlenecks hindering the maturation of flexible sensors and propose promising solutions. We first analyze challenges in achieving satisfactory sensing performance for real-world applications and then summarize issues in compatible sensor-biology interfaces, followed by brief discussions on powering and connecting sensor networks. Issues en route to commercialization and for sustainable growth of the sector are also analyzed, highlighting environmental concerns and emphasizing nontechnical issues such as business, regulatory, and ethical considerations. Additionally, we look at future intelligent flexible sensors. In proposing a comprehensive roadmap, we hope to steer research efforts towards common goals and to guide coordinated development strategies from disparate communities. Through such collaborative efforts, scientific breakthroughs can be made sooner and capitalized for the betterment of humanity.

Graphic abstract:

Organic semiconductor (OSC)-based gas detection has attracted considerable attention due to the facile manufacturing process and effective contact with target chemicals at room temperature. However, OSCs intrinsically suffer from inferior sensing and recovery capability due to lack of functional sites and deep gas penetration into the film. Here, we describe an interpenetrating polymer semiconductor nanonetwork (IPSN) channel possessing unreacted silanol (Si–OH) groups on its surface to overcome bottlenecks that come from OSC-based chemodetection. On the top of the IPSN, moreover, we introduced electron-donating amine (NH2) groups as a chemical receptor because they strongly interact with the electron-withdrawing nature of NO2gas. The NH2-IPSN-based field-effect transistor exhibited high-performance chemodetection such as ultrasensitivity (990% ppm–1at 5 ppm) and excellent NO2selectivity against other toxic gases. Impressively, the gas recovery was significantly improved because the NH2chemical receptors anchored on the surface of the IPSN suppress deep gas penetration into the film. This work demonstrates that our NO2chemodetection is expected to provide inspiration and guideline for realization of practical gas sensors in various industries and daily life.

We report an anion-sensing platform wherein conductance changes are triggered by chemical interactions between selectors and anions. The selector design incorporates both a cationic moiety (i.e., pyridinium) and a thiourea-based dual-hydrogen-bond donor. Anion binding by a model selector (2) was studied using 1H NMR and UV–vis titrations, which reveal a binding strength toward acetate ions (AcO–) followed by Cl–> Br–> NO3–. These studies reveal that selector 2is deprotonated upon addition of AcO–, whereas it undergoes hydrogen bonding associated with Cl–, Br–, and NO3–. The cationic pyridinium moiety improves anion binding affinity by lowering the pKavalue of selector 2and enhancing the hydrogen-bond donor capability as confirmed by spectroscopic titrations and DFT calculations. The selector is covalently attached to poly(4-vinylpyridine) (P4VP), which wraps single-walled carbon nanotubes (SWCNTs) (i.e., P4VP-2-SWCNT) to transduce an electrical signal. As a result, continuous anion sensing was achieved with high sensitivity represented by a normalized resistance change of 101.9 ± 10.3% toward 16.7 mM AcO–, whereas negligible sensitivity was observed toward Cl–, Br–, and NO3–. The sensitivity transition was attributed to the internal charge transfer of 2by deprotonation of the thiourea proton upon addition of AcO–.

Single-walled carbon nanotubes (SWCNTs) are recognized as versatile materials for the formation of chemiresistive sensors. However, imparting high sensitivity and selectivity to SWCNTs remains a major challenge. Herein, we report a new sensory system that interfaces SWCNTs and catalytic metal nanoparticles (NPs) in a film of a porous ion exchange polymer to produce sensitive and selective sensors. The porous polymer films are based on imidazolium-functionalized triptycene polyether sulfone, and the environment created by this polymer results in the formation of ultrasmall (<5 nm) Au NPs. The polymer serves to suppress the growth of Au NPs while maintaining gas transport. The size control promotes strong interactions between Au NPs and carbon monoxide (CO), and this composition produces a robust, sensitive, and selective CO chemiresistive sensor. We further demonstrate that the modulation of a gate voltage in chemical field-effect transistor sensing devices enhances the performance by promoting the activity of Au NPs. The sensors display an increase of CO response at room temperature in air under the negative gate voltage. Our results demonstrate that the combination of a porous ion exchange matrix, NPs, and gate voltage-modulated chemiresistors can be synergistically tuned to create sensitive and selective sensors for target analytes.

Biocompatible, electrically conductive microfibers with superior mechanical properties have received a great attention due to their potential applications in various biomedical applications such as implantable medical devices, biosensors, artificial muscles, and microactuators. Here, we developed an electrically conductive and mechanically stable carbon nanotube-based microactuator with a low degradability that makes it usable for an implantable device in the body or biological environments. The microfiber was composed of hyaluronic acid (HA) hydrogel and single-wall carbon nanotubes (SWCNTs) (HA/SWCNT). HA hydrogel acts as biosurfactant and ion-conducting binder to improve the dispersion of SWCNTs resulting in enhanced electrical and mechanical properties of the hybrid microfiber. In addition, HA was crosslinked to prevent the leaking of the nanotubes from the composite. Crosslinking of HA hydrogel significantly enhances Young’s modulus, the failure strain, the toughness, the stability of the electrical conductivity, and the resistance to biodegradation and creep of hybrid microfibers. The obtained crosslinked HA/SWCNT hybrid microfibers show an excellent capacitance and actuation behavior under mechanical loading with a low potential of ±1 V in a biological environment. Furthermore, the HA/SWCNT microfibers exhibit an excellent in vitro viability. Finally, the biocompatibility is shown through the resolution of an early inflammatory response in less than 3 weeks after the implantation of the microfibers in the subcutaneous tissue of mice.

The development of freestanding fiber-type chemiresistors, having high integration ability with various portable electronics including smart clothing systems, is highly demanding for the next-generation wearable sensing platforms. However, critical challenges stemming from the irreversible chemical sensing kinetics and weak reliability of the freestanding fiber-type chemiresistor hinder their practical use. In this work, for the first time, we report on the potential suitability of the freestanding and ultraporous reduced graphene oxide fiber functionalized with WO3nanorods (porous WO3NRs-RGO composite fiber) as a sensitive nitrogen dioxide (NO2) detector. By employing a tunicate cellulose nanofiber (TCNF), which is a unique animal-type cellulose, the numerous mesopores are formed on a wet-spun TCNF-GO composite fiber, unlike a bare GO fiber with dense surface structure. More interestingly, due to the superior wettability of TCNF, the aqueous tungsten precursor is uniformly adsorbed on an ultraporous TCNF-GO fiber, and subsequent heat treatment results in the thermal reduction of a TCNF-GO fiber and hierarchical growth of WO3NRs perpendicular to the porous RGO fiber (porous WO3NRs-RGO fiber). The freestanding porous WO3NRs-RGO fiber shows a notable response to 1 ppm NO2. Furthermore, we successfully demonstrate reversible NO2sensing characteristics of the porous WO3NRs-RGO fiber, which is integrated on a wrist-type wearable sensing device.

Real-time temperature monitoring of individual blood packages capable of wireless data transmission to ensure the safety of blood samples and minimize wastes has become a critical issue in recent years. In this work, we propose flexible temperature sensors using silver nanowires (NWs) and a flexible colorless polyimide (CPI) film integrated with a wireless data transmission circuit. The unique design of the temperature sensors was achieved by patterning Ag NWs using a three-dimensional printed mold and embedding the patterned Ag NWs in the CPI film (p-Ag NWs/CPI), which resulted in a flexible temperature sensor with electrical, mechanical, and temperature stability for applications in blood temperature monitoring. Indeed, a reliable resistance change of the p-Ag NWs/CPI was observed in the temperature range of −20 to 20 °C with a robust bending stability of up to 5000 cycles at 5 mm bending radius. Real-time and wireless temperature monitoring using the p-Ag NWs/CPI was demonstrated with the packages of rat blood. The result revealed that the stable and consistent temperature monitoring of individual blood packages could be achieved in a blood box, which was mainly attributed to the conformal attachment of the p-Ag NWs/CPI to different packages in a blood container.

We report a chemiresistive CO2sensor based on single-walled carbon nanotubes (SWCNTs) noncovalently functionalized with a CO2switchable copolymer containing amidine pendant groups that transform into amidinium bicarbonates in response to CO2. To fabricate a robust surface-anchored polymer–SWCNT dispersion via spray coating, we first designed and synthesized a precursor copolymer, P(4VP–VBAz), bearing both 4-vinylpyridine (4VP) groups and azide groups. The SWCNT dispersant group, 4VP, is capable of debundling and stabilizing nanotubes to improve their solubility in organic solvents for solution processing. Well-dispersed P(4VP–VBAz)–SWCNT composites are covalently immobilized onto a glass substrate functionalized with alkyl bromides, and then the amidine moieties are subsequently attached to form the resulting CO2-switchable P(Q4VP–VBAm)–SWCNT composites via a copper(I)-catalyzed azide–alkyne cycloaddition click reaction at the film surface. The amidine groups are strong donors that compensate or pin carriers in the SWCNTs. In the presence of CO2under humid conditions, the generated amidinium bicarbonates from the polymer wrapping increase the concentration and/or liberate the hole carriers in the nanotubes, thereby increasing the net conductance of the composites. The amidinium moieties revert back to the amidines when purged with a CO2-free carrier gas with a reversible decrease in conductance. We also demonstrate high selectivity to CO2over the other atmospheric gases such as O2and Ar.

Lead(II) acetate [Pb(Ac)2] reacts with hydrogen sulfide to form colored brownish precipitates of lead sulfide. Thus far, in order to detect leakage of H2S gas in industrial sectors, Pb(Ac)2has been used as an indicator in the form of test papers with a detection limit only as low as 5 ppm. Diagnosis of halitosis by exhaled breath needs sensors able to detect down to 1 ppm of H2S gas. In this work, high surface area and porous Pb(Ac)2anchored nanofibers (NFs) that overcome limitations of the conventional Pb(Ac)2-based H2S sensor are successfully achieved. First, lead(II) acetate, which melts at 75 °C, and polyacrylonitrile (PAN) polymer are mixed and stirred in dimethylformamide (DMF) solvent at 85 °C, enabling uniform dispersion of fine liquid droplets in the electrospinning solution. During the subsequent electrospinning, Pb(Ac)2anchored NFs are obtained, providing an ideal nanostructure with high thermal stability against particle aggregation, numerous reactions sites, and enhanced diffusion of H2S into the three-dimensional (3D)-networked NF web. This newly obtained sensing material can detect down to 400 ppb of H2S at a relative humidity of 90%, exhibiting high potential feasibility as a high-performance colorimetric sensor platform for diagnosis of halitosis.

Two-dimensional structures can potentially lead to not only modulation of electron transport but also the variations of optical property. Protonic ruthenium oxide, a two-dimensional atomic sheet material, has been synthesized, and its optoelectric properties have been investigated. The results indicate that protonic ruthenium oxide is an excellent candidate for use as a flexible, transparent conducting material. A hydrated-ruthenium-oxide sheet has been first prepared via the chemical exfoliation of sodium intercalated ruthenium oxide (NaRuO2) and, subsequently, converted into a protonic ruthenium oxide sheet using thermal treatment. A thermally activated transport mechanism is dominant in hydrated ruthenium oxide but diminishes in protonic ruthenium oxide; this resulted in a high electrical conductivity of ∼200 S/cm of the protonic sheet. Because of the unique interband and intraband structure, protonic ruthenium oxide has a small optical absorption coefficient of ∼1.62%/L. Consequently, such high conductivity and low absorption coefficient of protonic ruthenium oxide results in excellent transparent conducting properties.

Bimodally meso- (2–50 nm) and macroporous (>50 nm) WO3microbelts (MBs) functionalized with sub-3 nm Pt catalysts were fabricated via the electrospinning technique followed by subsequent calcination. Importantly, apoferritin (Apo), tea saponin and polystyrene colloid spheres (750 nm) dispersed in an electrospinning solution acted as forming agents for producing meso- and macropores on WO3MBs during calcination. Particularly, mesopores provide not only numerous reaction sites for effective chemical reactions, but also facilitate gas diffusion into the interior of the WO3MBs, dominated by Knudsen diffusion. The macropores further accelerate gas permeability in the interior and on the exterior of the WO3MBs. In addition, Pt nanoparticles with mean diameters of 2.27 nm were synthesized by using biological protein cages, such as Apo, to further enhance the gas sensing performance. Bimodally porous WO3MBs functionalized by Pt catalysts showed remarkably high hydrogen sulfide (H2S) response (Rair/Rgas= 61 @ 1 ppm) and superior selectivity to H2S against other interfering gases, such as acetone (CH3COCH3), ethanol (C2H5OH), ammonia (NH3), and carbon monoxide (CO). These results demonstrate a high potential for the feasibility of catalyst-loaded meso- and macroporous WO3MBs as new sensing platforms for the possibility of real-time diagnosis of halitosis.

Nanowire-transfer technology has received much attention thanks to its capability to fabricate high-performance flexible nanodevices with high simplicity and throughput. However, it is still challenging to extend the conventional nanowire-transfer method to the fabrication of a wide range of devices since a chemical-adhesion-based nanowire-transfer mechanism is complex and time-consuming, hindering successful transfer of diverse nanowires made of various materials. Here, we introduce a material-independent mechanical-interlocking-based nanowire-transfer (MINT) method, fabricating ultralong and fully aligned nanowires on a large flexible substrate (2.5 × 2 cm2) in a highly robust manner. For the material-independent nanotransfer, we developed a mechanics-based nanotransfer method, which employs a dry-removable amorphous carbon (a-C) sacrificial layer between a vacuum-deposited nanowire and the underlying master mold. The controlled etching of the sacrificial layer enables the formation of a mechanical-interlocking structure under the nanowire, facilitating peeling off of the nanowire from the master mold robustly and reliably. Using the developed MINT method, we successfully fabricated various metallic and semiconductor nanowire arrays on flexible substrates. We further demonstrated that the developed method is well suited to the reliable fabrication of highly flexible and high-performance nanoelectronic devices. As examples, a fully aligned gold (Au) microheater array exhibited high bending stability (106cycling) and ultrafast (∼220 ms) heating operation up to ∼100 °C. An ultralong Au heater-embedded cuprous-oxide (Cu2O) nanowire chemical gas sensor showed significantly improved reversible reaction kinetics toward NO2with 10-fold enhancement in sensitivity at 100 °C.

Two-dimensional (2D) nanostructures are gaining tremendous interests due to the fascinating physical, chemical, electrical, and optical properties. Recent advances in 2D nanomaterials synthesis have contributed to optimization of various parameters such as physical dimension and chemical structure for specific applications. In particular, development of high performance gas sensors is gaining vast importance for real-time and on-site environmental monitoring by detection of hazardous chemical species. In this review, we comprehensively report recent achievements of 2D nanostructured materials for chemiresistive-type gas sensors. Firstly, the basic sensing mechanism is described based on charge transfer behavior between gas species and 2D nanomaterials. Secondly, diverse synthesis strategies and characteristic gas sensing properties of 2D nanostructures such as graphene, metal oxides, transition metal dichalcogenides (TMDs), metal organic frameworks (MOFs), phosphorus, and MXenes are presented. In addition, recent trends in synthesis of 2D heterostructures by integrating two different types of 2D nanomaterials and their gas sensing properties are discussed. Finally, this review provides perspectives and future research directions for gas sensor technology using various 2D nanomaterials.

Metal nanowires have been considered as essential components for flexible transparent conducting electrodes (TCEs) with high transparency and low sheet resistance. However, large surface roughness and high interwire junction resistance limit the practical use of metal wires as TCEs. Here, we report Cu microbelt network (Cu MBN) with coalescence junction and low surface roughness for next-generation flexible TCEs. In particular, the unique embedded structure of Cu MBN in colorless polyimide (cPI) film was achieved to reduce the surface roughness as well as enhance mechanical stability. The TCEs using junction-free Cu MBN embedded in cPI exhibited excellent mechanical stability up to 100 000 bending cycles, high transparency of 95.18%, and a low sheet resistance of 6.25 Ω sq–1. Highly robust Cu MBN-embedded cPI-based TCE showed outstanding flexible heater performance, i.e., high saturation temperature (120 °C) at very low voltage (2.3 V), owing to the high thermal stability of cPI and excellent thermal conductivity of the Cu MBN.

Pd based alloy materials with hollow nanostructures are ideal hydrogen (H2) sensor building blocks because of their double-H2sensing active sites (interior and exterior side of hollow Pd alloy) and fast response. In this work, for the first time, we report a simple fabrication process for preparing hollow Pd–Ag alloy nanowires (Pd@Ag HNWs) by using the electrodeposition of lithographically patterned silver nanowires (NWs), followed by galvanic replacement reaction (GRR) to form palladium. By controlling the GRR time of aligned Ag NWs within an aqueous Pd2+-containing solution, the compositional transition and morphological evolution from Ag NWs to Pd@Ag HNWs simultaneously occurred, and the relative atomic ratio between Pd and Ag was controlled. Interestingly, a GRR duration of 17 h transformed Ag NWs into Pd@Ag HNWs that showed enhanced H2response and faster sensing response time, reduced 2.5-fold, as compared with Ag NWs subjected to a shorter GRR period of 10 h. Furthermore, Pd@Ag HNWs patterned on the colorless and flexible polyimide (cPI) substrate showed highly reversible H2sensing characteristics. To further demonstrate the potential use of Pd@Ag HNWs as sensing layers for all-transparent, wearable H2sensing devices, we patterned the Au NWs perpendicular to Pd@Ag HNWs to form a heterogeneous grid-type metallic NW electrode which showed reversible H2sensing properties in both bent and flat states.

Detection and control of air quality are major concerns in recent years for environmental monitoring and healthcare. In this work, we developed an integrated sensor architecture comprised of nanostructured composite sensing layers and a flexible heating substrate for portable and real-time detection of nitrogen dioxide (NO2). As sensing layers, PdO-infiltrated Co3O4hollow nanocubes (PdO-Co3O4HNCs) were prepared by calcination of Pd-embedded Co-based metal–organic framework polyhedron particles. Single-walled carbon nanotubes (SWCNTs) were functionalized with PdO-Co3O4HNCs to control conductivity of sensing layers. As a flexible heating substrate, the Ni mesh electrode covered with a 40 nm thick Au layer (i.e., Ni(core)/Au(shell) mesh) was embedded in a colorless polyimide (cPI) film. As a result, SWCNT-functionalized PdO-Co3O4HNCs sensor exhibited improved NO2detection property at 100 °C, with high sensitivity (S) of 44.11% at 20 ppm and a low detection limit of 1 ppm. The accelerated reaction and recovery kinetics toward NO2of SWCNT-functionalized PdO-Co3O4HNCs were achieved by generating heat on the Ni(core)/Au(shell) mesh-embedded cPI substrate. The SWCNT-functionalized porous metal oxide sensing layers integrated on the mechanically stable Ni(core)/Au(shell) mesh heating substrate can be envisioned as an essential sensing platform for realization of low-temperature operation wearable chemical sensor.

We present a fast, energy-efficient nano-thermomechanical encoding scheme for digital information storage and retrieval. Digital encoding processes are conducted by the bistable electrothermal actuation of a scalable nanobridge device. The electrothermal energy is highly concentrated by enhanced electron/phonon scattering and heat insulation in a sub-100 nm metallic layer. The efficient conversion of electrothermal energy into mechanical strain allows digital switching and programming processes within 60 ns at 0.75 V with a programming energy of only 54 pJ. Furthermore, this encoding scheme together with the thermally robust design enables data retention at temperatures up to 400 °C. These results suggest that the proposed nano-thermomechanical encoding method could contribute to low-power electronics and robust information storage/retrieval systems.

Room-temperature (RT) operation sensors are constantly in increasing demand because of their low power consumption, simple operation, and long lifetime. However, critical challenges such as low sensing performance, vulnerability under highly humid state, and poor recyclability hinder their commercialization. In this work, sub-10 nm hollow, bimetallic Pt–Ag nanoparticles (NPs) were successfully formed by galvanic replacement reaction in bioinspired hollow protein templates and sensitized on the multidimensional SnO2–WO3heterojunction nanofibers (HNFs). Formation of hollow, bimetallic NPs resulted in the double-side catalytic effect, rendering both surface and inner side chemical reactions. Subsequently, SnO2–WO3HNFs were synthesized by incorporating 2D WO3nanosheets (NSs) with 0D SnO2sphere by c-axis growth inhibition effect and fluid dynamics of liquid Sn during calcination. Hierarchically assembled HNFs effectively modulate surface depletion layer of 2D WO3NSs by electron transfers from WO3to SnO2stemming from creation of heterojunction. Careful combination of bimetallic catalyst NPs with HNFs provided an extreme recyclability under exhaled breath (95 RH%) with outstanding H2S sensitivity. Such sensing platform clearly distinguished between the breath of healthy people and simulated halitosis patients.

Metal–organic framework (MOF)-derived synergistic catalysts were easily functionalized on hollow SnO2nanotubes (NTs) via electrospinning and subsequent calcination. Nanoscale Pd NPs (∼2 nm) loaded Zn-based zeolite imidazole framework (Pd@ZIF-8, ∼80 nm) was used as a new catalyst-loading platform for the effective functionalization of a PdO@ZnO complex catalyst onto the thin wall of one-dimensional metal oxide NTs. The well-dispersed nanoscale PdO catalysts (3–4 nm) and multiheterojunctions (PdO/ZnO and ZnO/SnO2) on hollow structures are essential for the development of high-performance gas sensors. As a result, the PdO@ZnO dual catalysts-loaded hollow SnO2NTs (PdO@ZnO–SnO2NTs) exhibited high acetone response (Rair/Rgas= 5.06 at 400 °C @ 1 ppm), superior acetone selectivity against other interfering gases, and fast response (20 s) and recovery (64 s) time under highly humid atmosphere (95% RH). In this work, the advantages of hollow SnO2NT structures with high surface area and open porosity were clearly demonstrated by the comparison to SnO2nanofibers (NFs). Moreover, the sensor arrays composed of SnO2NFs, SnO2NTs, PdO@ZnO–SnO2NFs, and PdO@ZnO–SnO2NTs successfully identified the patterns of the exhaled breath of normal people and simulated diabetics by using a principal component analysis.

The increase of surface area and the functionalization of catalyst are crucial to development of high-performance semiconductor metal oxide (SMO) based chemiresistive gas sensors. Herein, nanoscale catalyst loaded Co3O4hollow nanocages (HNCs) by using metal–organic framework (MOF) templates have been developed as a new sensing platform. Nanoscale Pd nanoparticles (NPs) were easily loaded on the cavity of Co based zeolite imidazole framework (ZIF-67). The porous structure of ZIF-67 can restrict the size of Pd NPs (2–3 nm) and separate Pd NPs from each other. Subsequently, the calcination of Pd loaded ZIF-67 produced the catalytic PdO NPs functionalized Co3O4HNCs (PdO–Co3O4HNCs). The ultrasmall PdO NPs (3–4 nm) are well-distributed in the wall of Co3O4HNCs, the unique structure of which can provide high surface area and high catalytic activity. As a result, the PdO–Co3O4HNCs exhibited improved acetone sensing response (Rgas/Rair= 2.51–5 ppm) compared to PdO–Co3O4powders (Rgas/Rair= 1.98), Co3O4HNCs (Rgas/Rair= 1.96), and Co3O4powders (Rgas/Rair= 1.45). In addition, the PdO–Co3O4HNCs showed high acetone selectivity against other interfering gases. Moreover, the sensor array clearly distinguished simulated exhaled breath of diabetics from healthy people’s breath. These results confirmed the novel synthesis of MOF templated nanoscale catalyst loaded SMO HNCs for high performance gas sensors.

Highly selective detection, rapid response (<20 s), and superior sensitivity (Rair/Rgas> 50) against specific target gases, particularly at the 1 ppm level, still remain considerable challenges in gas sensor applications. We propose a rational design and facile synthesis concept for achieving exceptionally sensitive and selective detection of trace target biomarkers in exhaled human breath using a protein nanocage templating route for sensitizing electrospun nanofibers (NFs). The mesoporous WO3NFs, functionalized with well-dispersed nanoscale Pt, Pd, and Rh catalytic nanoparticles (NPs), exhibit excellent sensing performance, even at parts per billion level concentrations of gases in a humid atmosphere. Functionalized WO3NFs with nanoscale catalysts are demonstrated to show great promise for the reliable diagnosis of diseases.

Diagnostic sensing device using exhaled breath of human have critical advantages due to the noninvasive diagnosis and high potential for portable device with simple analysis process. Here, we report ultrafast as well as highly sensitive bumpy WO3hemitube nanostructure assisted by O2plasma surface modification with functionalization of graphene-based material for the detection of acetone (CH3COCH3) and hydrogen sulfide (H2S) which are biomarkers for the diagnosis of diabetes and halitosis, respectively. 0.1 wt % graphene oxide (GO)- and 0.1 wt % thin layered graphite (GR)- WO3hemitube composites showed response times of 11.5 ± 2.5 s and 13.5 ± 3.4 s to 1 ppm acetone as well as 12.5 ± 1.9 s and 10.0 ± 1.6 s to 1 ppm of H2S, respectively. In addition, low limits of detection (LOD) of 100 ppb (Rair/Rgas= 1.7 for acetone and Rair/Rgas= 3.3 for H2S at 300 °C) were achieved. The superior sensing properties were ascribed to the electronic sensitization of graphene based materials by modulating space charged layers at the interfaces between n-type WO3hemitubes and p-type graphene based materials, as identified by Kelvin Probe Force Microscopy (KPFM). Rapid response and superior sensitivity of the proposed sensing materials following cyclic thermal aging demonstrates good potential for real-time exhaled breath diagnosis of diseases.

Sensitive detection of acetone and hydrogen sulfide levels in exhaled human breath, serving as breath markers for some diseases such as diabetes and halitosis, may offer useful information for early diagnosis of these diseases. Exhaled breath analyzers using semiconductor metal oxide (SMO) gas sensors have attracted much attention because they offer low cost fabrication, miniaturization, and integration into portable devices for noninvasive medical diagnosis. However, SMO gas sensors often display cross sensitivity to interfering species. Therefore, selective real-time detection of specific disease markers is a major challenge that must be overcome to ensure reliable breath analysis. In this work, we report on highly sensitive and selective acetone and hydrogen sulfide detection achieved by sensitizing electrospun SnO2nanofibers with reduced graphene oxide (RGO) nanosheets. SnO2nanofibers mixed with a small amount (0.01 wt %) of RGO nanosheets exhibited sensitive response to hydrogen sulfide (Rair/Rgas= 34 at 5 ppm) at 200 °C, whereas sensitive acetone detection (Rair/Rgas= 10 at 5 ppm) was achieved by increasing the RGO loading to 5 wt % and raising the operation temperature to 350 °C. The detection limit of these sensors is predicted to be as low as 1 ppm for hydrogen sulfide and 100 ppb for acetone, respectively. These concentrations are much lower than in the exhaled breath of healthy people. This demonstrates that optimization of the RGO loading and the operation temperature of RGO–SnO2nanocomposite gas sensors enables highly sensitive and selective detection of breath markers for the diagnosis of diabetes and halitosis.

Optically reduced graphene oxide (RGO) sheets were produced on a thermally stable and highly transparent colorless polyimide (CPI) substrate by irradiating intense pulsed light (IPL) on a GO-coated CPI film. These RGO sheets can be used as flexible gas sensing layers for wearable applications. Ultrafast IPL irradiation formed RGO sheets on the CPI film within 4 msec without any damage on the plastic substrate. The IPL-induced RGO (IPL-RGO) sheets exhibited dramatically improved chemical sensing performance toward H2S, C2H5OH, and H2, while the pristine GO sheets did not show any gas responses. In addition, consistent sensing properties were maintained even after the IPL-RGO sheets on the CPI film were mechanically deformed for 104bending cycles. The gas responses of an IPL-RGO sensor toward H2S, C2H5OH and H2were clearly distinguished by pattern recognition based on principal component analysis. Moreover, we successfully integrated our IPL-RGO sensor on a flexible printed circuit board with wireless Bluetooth communication and demonstrated outstanding sensing properties for potential applications in environmental and healthcare monitoring.