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Atmospheric NO2 is of great concern due to its adverse effects on human health and the environment, motivating research on NO2 detection and remediation. Existing low-cost room-temperature NO2 sensors often suffer from low sensitivity at the ppb level or long recovery times, reflecting the trade-off between sensor response and recovery time. Here, we report an atomically dispersed metal ion strategy to address it. We discover that bimetallic PbCdSe quantum dot (QD) gels containing atomically dispersed Pb ionic sites achieve the optimal combination of strong sensor response and fast recovery, leading to a high-performance room-temperature p-type semiconductor NO2 sensor as characterized by a combination of ultra–low limit of detection, high sensitivity and stability, fast response and recovery. With the help of theoretical calculations, we reveal the high performance of the PbCdSe QD gel arises from the unique tuning effects of Pb ionic sites on NO2 binding at their neighboring Cd sites. Quantum dot-based NO2 sensors often suffer from low sensitivity or long recovery times. Here, the authors report that bimetallic PbCdSe quantum dot gels containing atomically dispersed Pb ionic sites enable ultra-sensitive and fast NO2 sensing. [ABSTRACT FROM AUTHOR]

Slow response and recovery kinetics is a major challenge for practical room-temperature NO 2 gas sensing. Here, we report the use of visible light illumination to significantly shorten the response and recovery times of a PbSe quantum dot (QD) gel sensor by 21% (to 27 s) and 63% (to 102 s), respectively. When combined with its high response (0.04%/ppb) and ultralow limit of detection (3 ppb), the reduction in response and recovery time makes the PbSe QD gel sensor among the best p-type room-temperature NO 2 sensors reported to date. A combined experimental and theoretical investigation reveals that the accelerated response and recovery time is primarily due to photoexcitation of NO 2 gaseous molecules and adsorbed NO 2 on the gel surface, rather than the excitation of the semiconductor sensing material, as suggested by the currently prevailing light-activated gas-sensing theory. Furthermore, we find that the extent of improvement attained in the recovery speed also depends on the distribution of excited electrons in the adsorbed NO 2 /QD gel system. This work suggests that the design of light-activated sensor platforms may benefit from a careful assessment of the photophysics of the analyte in the gas phase and when adsorbed onto the semiconductor surface.