Hydrogen (H 2 ) is one of the next-generation energy sources because it is abundant in nature and has a high combustion efficiency that produces environmentally benign products (H 2 O). However, H 2 /air mixtures are explosive at H 2 concentrations above 4%, thus any leakage of H 2 must be rapidly and reliably detected at much lower concentrations to ensure safety. Among the various types of H 2 sensors, chemiresistive sensors are one of the most promising sensing systems due to their simplicity and low cost. This review highlights the advances in H 2 chemiresistors, including metal-, semiconducting metal oxide-, carbon-based materials, and other materials. The underlying sensing mechanisms for different types of materials are discussed, and the correlation of sensing performances with nanostructures, surface chemistry, and electronic properties is presented. In addition, the discussion of each material emphasizes key advances and strategies to develop superior H 2 sensors. Furthermore, recent key advances in other types of H 2 sensors are briefly discussed. Finally, the review concludes with a brief outlook, perspective, and future directions.

Edges of 2D transition metal dichalcogenides (TMDs) are well known as highly reactive sites, thus researchers have attempted to maximize the edge site density of 2D TMDs. In this work, metal-organic framework (MOF) templates are introduced to synthesize few-layered WS 2 nanoplates (a lateral dimension of ≈10 nm) confined in Co, N-doped hollow carbon nanocages (WS 2 _Co-N-HCNCs), for highly sensitive NO 2 gas sensors. WS 2 precursors are assembled in the surface cavity of Co-based zeolite imidazole framework (ZIF-67) and subsequent pyrolysis produced WS 2 _Co-N-HCNCs. During the pyrolysis, the carbonized ZIF-67 are doped by Co and N elements, and the growth of WS 2 is effectively suppressed, creating few-layered WS 2 nanoplates functionalized Co-N-HCNCs. The WS 2 _Co-N-HCNCs exhibit outstanding NO 2 sensing characteristics at room temperature, in terms of response (48.2% to 5 ppm), selectivity, response and recovery speed, and detection limit (100 ppb). These results are attributed to the enhanced adsorption and desorption kinetics of NO 2 on abundant WS 2 edges, confined in the gas permeable HCNCs. This work opens up an efficient way for the facile synthesis of edge abundant few-layered TMDs combined with porous carbon matrix via MOF templating route, for applications relying on highly active sites.

Catalysis with single-atom catalysts (SACs) exhibits outstanding reactivity and selectivity. However, fabrication of supports for the single atoms with structural versatility remains a challenge to be overcome, for further steps toward catalytic activity augmentation. Here, we demonstrate an effective synthetic approach for a Pt SAC stabilized on a controllable one-dimensional (1D) metal oxide nano-heterostructure support, by trapping the single atoms at heterojunctions of a carbon nitride/SnO2 heterostructure. With the ultrahigh specific surface area (54.29 m2 g–1) of the nanostructure, we obtained maximized catalytic active sites, as well as further catalytic enhancement achieved with the heterojunction between carbon nitride and SnO2. X-ray absorption fine structure analysis and HAADF-STEM analysis reveal a homogeneous atomic dispersion of Pt species between carbon nitride and SnO2 nanograins. This Pt SAC system with the 1D nano-heterostructure support exhibits high sensitivity and selectivity toward detection of formaldehyde gas among state-of-the-art gas sensors. Further ex situ TEM analysis confirms excellent thermal stability and sinter resistance of the heterojunction-immobilized Pt single atoms.

The colorimetric gas sensor offers an opportunity for the simple and rapid detection of toxic gaseous substances based on visually discernible changes in the color of the sensing material. In particular, the accurate detection of trace amounts of certain biomarkers in a patient's breath provides substantial clues regarding specific diseases, for example, hydrogen sulfide (H 2 S) for halitosis and ammonia (NH 3 ) for kidney disorder. However, conventional colorimetric sensors often lack the sensitivity, selectivity, detection limit, and mass-productivity, impeding their commercialization. Herein, we report an inexpensive route for the meter-scale synthesis of a colorimetric sensor based on a composite nanofiber yarn that is chemically functionalized with an ionic liquid as an effective H 2 S adsorbent and lead acetate as a colorimetric dye. As an eyereadable and weavable sensing platform, the single-strand yarn exhibits enhanced sensitivity supported by its high surface area and well-developed porosity to detect the breath biomarker (1 ppm of H 2 S). Alternatively, the yarn loaded with lead iodide dyes could reversibly detect NH 3 gas molecules in the ppm-level, demonstrating the facile extensibility. Finally, we demonstrated that the freestanding yarns could be sewn into patterned textiles for the fabrication of a wearable toxic gas alarm system with a visual output.

Conductive porous materials having a high surface reactivity offer great promise for a broad range of applications. However, a general and scalable synthesis of such materials remains challenging. In this work, the facile synthesis of catalytic metal nanoparticles (NPs) embedded in 2D metal–organic frameworks (MOFs) is reported as highly active and conductive porous materials. After the assembly of 2D conductive MOFs (C‐MOFs), i.e., Cu3(hexahydroxytriphenylene)2 [Cu3(HHTP)2], Pd or Pt NPs are functionalized within the cavities of C‐MOFs by infiltration of metal ions and subsequent reduction. The unique structure of Cu3(HHTP)2 with a cavity size of 2 nm confines the bulk growth of metal NPs, resulting in ultra‐small (≈2 nm) and well‐dispersed metal NPs loaded in 2D C‐MOFs. The Pd or Pt NPs‐loaded Cu3(HHTP)2 exhibits remarkably improved NO2 sensing performance at room temperature due to the high reactivity of catalytic metal NPs and the high porosity of C‐MOFs. The catalytic effect of Pd and Pt NPs on NO2 sensing of Cu3(HHTP)2, in terms of reaction rate kinetics and activation energy, is demonstrated.

Continuous monitoring of hydrogen sulfide (H2S) in human breath for early stage diagnosis of halitosis is of great significance for prevention of dental diseases. However, fabrication of a highly selective and sensitive H2S gas sensor material still remains a challenge, and direct analysis of real breath samples has not been properly attempted, to the best of our knowledge. To address the issue, herein, we introduce facile cofunctionalization of WO3 nanofibers with alkaline metal (Na) and noble metal (Pt) catalysts via the simple addition of sodium chloride (NaCl) and Pt nanoparticles (NPs), followed by electrospinning process. The Na-doping and Pt NPs decoration in WO3 grains induces the partial evolution of the Na2W4O13 phase, causing the buildup of Pt/Na2W4O13/WO3 multi-interface heterojunctions that selectively interacts with sulfur-containing species. As a result, we achieved the highest-ranked sensing performances, that is, response (R air/R gas) = 780 @ 1 ppm and selectivity (R H2S/R EtOH) = 277 against 1 ppm ethanol, among the chemiresistor-based H2S sensors, owing to the synergistic chemical and electronic sensitization effects of the Pt NP/Na compound cocatalysts. The as-prepared sensing layer was proven to be practically effective for direct, and quantitative halitosis analysis based on the correlation (accuracy = 86.3%) between the H2S concentration measured using the direct breath signals obtained by our test device (80 cases) and gas chromatography. This study offers possibilities for direct, highly reliable and rapid detection of H2S in real human breath without the need of any collection or filtering equipment.

PtO nanocatalysts-loaded SnO multichannel nanofibers (PtO-SnO MCNFs) were synthesized by single-spinneret electrospinning combined with apoferritin and two immiscible polymers, i.e., poly(vinylpyrrolidone) and polyacrylonitrile. The apoferritin, which can encapsulate nanoparticles within a small inner cavity (8 nm), was used as a catalyst loading template for an effective functionalization of the PtO catalysts. Taking advantage of the multichannel structure with a high porosity, effective activation of catalysts on both interior and exterior site of MCNFs was realized. As a result, under high humidity condition (95% RH), PtO-SnO MCNFs exhibited a remarkably high acetone response (R/R = 194.15) toward 5 ppm acetone gases, superior selectivity to acetone molecules among various interfering gas species, and excellent stability during 30 cycles of response and recovery toward 1 ppm acetone gases. In this work, we first demonstrate the high suitability of multichannel semiconducting metal oxides structure functionalized by apoferritin-encapsulated catalytic nanoparticles as highly sensitive and selective gas-sensing layer.

Although single-nozzle electrospraying seems a versatile technique in the synthesis of spherical semiconducting metal oxide structures, the synthesized structures find limited use in gas-sensing applications because of their thick and dense morphology, which minimizes the accessibility of their inner surfaces. Herein, unprecedented spherical SiO@SnO core-shell structures are synthesized upon calcination of single-nozzle as-electrosprayed spheres (SPs) containing tin (Sn) and silicon (Si) precursors. Subsequent etching of SiO in NaOH (pH 12) affords meso/macroporous SnO hollow spheres (HSPs) with short diffusion length (31.4 ± 3.1 nm), small crystallites (15.5 nm), and large Brunauer-Emmett-Teller surface area (124.8 m g). Apart from surface meso/macropores, diffusion of gases into porous SnO sensing layers is realized through inner interconnection of voids of the SnO HSPs into a three-dimensional network. Functionalization of the postetched SnO HSPs with platinum (Pt) nanoparticles at 0.08 wt % yields gas-sensing materials with outstanding response ( R/ R = 1.6, 10.8, and 105.1-0.1, 1, and 5 ppm of HS, respectively) and selectivity toward HS against interfering gas molecules at 250 °C. The SiO phase in the postcalcined SiO@SnO SPs acts as a sacrificial template for pore creation and crystal growth inhibition, whereas the small amount of SiO residues in HSPs enhances the selectivity.