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Yttria-stabilized zirconia (YSZ) based potentiometric gas sensors have been widely utilized for detecting NOx (NO and NO2). Nevertheless, it is still remains challenging issue for YSZ-based sensors to sense total NOx due to the opposite response signals to NO and NO2. Herein, we report an efficient strategy to sense total NOx at high temperature (above 300 °C) by designing a dual functional sensing electrode (SE); namely, the SE will simultaneously convert NO (in NOx mixture) to NO2 and electrocatalyze all of the obtained NO2 to generate the response signal of total NOx. In comparison with those previously reported total NOx sensors, the proposed total NOx sensor will be featured with a simplified sensor configuration and desirable long-term stability. To confirm the practicability of the proposed strategy, the NO conversion rate of several metal oxides and their composites have been measured and it turns out that the Co3O4/NiO shows relatively high NO conversion rate. Further study indicates a YSZ-based sensor consisting of (Co3O4 + 20 wt % NiO)-SE and Mn-based RE demonstrates satisfactory performance in detecting total NOx. For instance, analogous response magnitude to NO and NO2 as well as the mixture of NO/NO2 (within 35 ppm) is witnessed for the sensor; particularly, the sensor gives acceptable stability and response/recovery rate at the operating temperature of 500 °C within the examined period. In summary, the use of dual functional SE (e.g., Co3O4/NiO composite SE) indeed addressed those issues of concern in monitoring the level of total NOx and has provided a promising alternative way for designing future high-performance total NOx sensor.

During the detection of industrial toxic gases, such as triethylamine (TEA), poor selectivity and negative humidity impact are still challenging issues. A frequently reported strategy is to employ molecular sieves or metal-organic framework (MOF) membranes so that interference derived from surrounding gases or water vapor can be blocked. Nevertheless, the decline in the response signal was also observed after coating these membranes. Herein, an alternative strategy that is based on a hydrophobic, TEA adsorption-selective p-n conjunction core-shell heterostructure is proposed and is speculated to simultaneously enhance selectivity, sensitivity, and humidity resistance. To verify the practicability of the proposed strategy, a thickness-tunable nitrogen-doped carbon (N-C) shell-coated α-Fe2O3 nano-olive (N-C@α-Fe2O3 NO)-based core-shell heterostructure that is obtained via a unique all-vapor-phase processing method is selected as the research example. After forming the core-shell heterostructure, a relatively hydrophobic and TEA adsorption-selective N-C@α-Fe2O3 NO surface was experimentally confirmed. Particularly, a chemiresistive sensor that comprises N-C@α-Fe2O3 NOs exhibits satisfactory selectivity and response magnitude to TEA when compared with the sensor using α-Fe2O3 NOs. The detection limit can even reduce to be 400 ppb at 250 °C. Furthermore, the sensor based on N-C@α-Fe2O3 NOs shows desirable humidity resistance within the relative humidity (RH) range of 30-90%. For practical usage, a sensing prototype based on the N-C@α-Fe2O3 NO probe is fabricated, and its satisfactory sensing performance further confirms the potential for future applications in industrial organic amine detection. These promising results show a bright future in enhancing the humidity resistance and selectivity as well as sensitivity of chemiresistive sensors by simply designing a hydrophobic and target gas adsorption (e.g., TEA) preferred p-n junction core-shell heterostructure.

Breath analysis has been considered a noninvasive, safe, and reliable way to diagnose cancer at very early stage. Rapid detection of cancer volatile markers in breath samples via a portable sensing device will lay the foundation of future early cancer diagnosis. Nevertheless, unsatisfactory sensitivity and specificity of these sensing devices restrain the clinical application of breath analysis. Herein, we proposed the strategy of designing the light-regulated electrochemical reaction assisted core-shell heterostructure to address the issue of concern; that is, the photoactive shell will be designed for trigging the light-regulated electrochemical reaction and enhancing the sensitivity while a catalytic active core will play the function of removing interference gases. After screening of various core candidates, Fe2O3 was found to exhibit relatively low conversion rate to 3-methylhexane, which is one of the representative volatile markers for breath analysis, suggesting that mutual interference would be eliminated by Fe2O3. Based on this assumption, an electrochemical sensor comprising core-shell Fe2O3@ZnO-SE (vs Mn-based RE) was fabricated and sensing properties to 6 kinds of volatile markers was evaluated. Interestingly, the thickness of ZnO shell significantly influenced the response behavior; typically, the Fe2O3@ZnO with shell thickness of 4.8 nm offers the sensor high selectivity to 3-methylhexane. In contrast, significantly mutual response interference is observed for the Fe2O3@ZnO with extremely thick/thin shell. Particularly, sensing properties are greatly enhanced upon illumination; a detection limit to 3-methylhexane can even be as low as 0.072 ppm which will be useful in clinic application. Besides, the high selectivity of the sensor to 3-methylhexane is further confirmed by the testing of simulated breath samples. In summary, we anticipate that the strategy proposed in this research will be a starting point for artificially tailoring the sensitivity and selectivity of future sensing devices.